REVIEW OF THE AIR QUALITY DIRECTIVE AND THE 4 TH DAUGHTER DIRECTIVE

Transcription

1 REVIEW OF THE AIR QUALITY DIRECTIVE AND THE 4 TH DAUGHTER DIRECTIVE Support Services for the implementation of Art. 32 of AQD and Art. 8 of 4 th DD Service Request No. 6 under framework contract ENV.C.3/FRA/2009/0008 Final report Iris Buxbaum Beth Conlan Chris Conolly Sally Cooke Brian Donovan Marina Fröhlich Dick van den Hout Lorenz Moosmann Christian Nagl Jürgen Schneider Wolfgang Spangl Brian Stacey John Stedman Marita Voogt Brigitte Winter Vienna, 23 February 2013

2 Project management Christian Nagl Authors Iris Buxbaum, Umweltbundesamt Beth Conlan, Ricardo - AEA Chris Conolly, Ricardo AEA Sally Cooke, Ricardo AEA Brian Donovan, Ricardo AEA Marina Fröhlich, Umweltbundesamt Dick van den Hout, TNO Lorenz Moosmann, Umweltbundesamt Christian Nagl, Umweltbundesamt Jürgen Schneider, Umweltbundesamt Wolfgang Spangl, Umweltbundesamt Brian Stacey, Ricardo AEA John Stedman, Ricardo AEA Marita Voogt, TNO Brigitte Winter, Umweltbundesamt Review Task 1: Lorenz Moosmann, Umweltbundesamt Christian Nagl, Umweltbundesamt Wolfgang Spangl, Umweltbundesamt Task 2: Iris Buxbaum, Umweltbundesamt Brian Donovan, Ricardo AEA Marina Fröhlich, Umweltbundesamt Christian Nagl, Umweltbundesamt Wolfgang Spangl, Umweltbundesamt Brian Stacey, Ricardo AEA Marita Voogt, TNO Task 3: Christian Nagl, Umweltbundesamt Jürgen Schneider, Umweltbundesamt Wolfgang Spangl, Umweltbundesamt Task 4: Beth Conlan, Ricardo AEA Sally Cooke, Ricardo AEA Brian Stacey, Ricardo AEA John Stedman, Ricardo AEA Task 5: Dick van den Hout, TNO Disclaimer The orientation and content of this report cannot be taken as indicating the position of the European Commission or its services. For further information about the publications of the Umweltbundesamt please go to:

3 Service Request 6 final report Content CONTENT SUMMARY INTRODUCTION ASSESSMENT OF CURRENT AQ SITUATIONS, PROJECTIONS, REDUCTION POTENTIALS Key messages Introduction Basis Data sources Comparison of monitoring data with limit values, target values and assessment thresholds Report Structure Work covered by this task PM PM Analysis of current (2010) ambient PM 2.5 annual mean concentrations Analysis of historic trends in ambient PM 2.5 concentrations Analysis of historic trends in emission of PM Calculation and assessment of the Average Exposure Indicator (AEI) PM below PM 2.5 and constituents Nickel Cadmium Arsenic Benzo(a)pyrene Mercury Reduction potentials REVIEW OF ASSESSMENT METHODOLOGIES FOR РM 10, PM 2.5, HEAVY METALS AND PAHS Key messages Context Scope and general approach Review information provided Does the data provided show inconsistencies which may be related to technical monitoring issues? Do the datasets provided fulfil the basic requirements of the directives (data capture, QA/QC, etc)? Is there any other monitoring undertaken by the member states (additional sites or additional pollutants) that is not submitted to DEM? Umweltbundesamt Vienna, 23 February

4 Service Request 6 final report Content 3.5 Evaluate data quality objectives Analysis of reports available from network operators, including reports on equivalence testing Recommendations for improvements Siting criteria Reference methods Reference methods for PM Reference methods for total gaseous mercury and heavy metals and PAH in PM Deposition of heavy metals and PAH PM 10 vs. PM Which PM fraction is the most relevant from the point of view of documented health effects? Is it feasible for monitoring network operators to monitor both fractions, taking into account the availability of new monitoring techniques? Is particle number a better metric than particle mass with respect to human health? Is there a need for new reference methods? Conclusions Reference method vs. near-real-time information Are there any implications associated with the fact that there is no standard method for continuous PM monitoring? Is there any information to suggest that the relationships between continuous and gravimetric samplers remains constant with time? Does this render information to the public more difficult? What would be the advantages/disadvantages of a separate, continuous standard method? Particle size fractions Benzo(a)pyrene as marker Relationships between pollutants DEVELOPING FUTURE OBJECTIVE(S) FOR PM Key messages Context Identification possible new PM standards and selection for further investigation Criteria for air quality standards Selection of possible new PM standards for further investigation PM fraction Evaluating the current state of implementation of the relevant provisions Implementation of assessment provisions Implementation of management provisions Questionnaire on air quality management for PM 2.5 reduction targets and exposure obligation Overview of current levels, projections, reduction potential and technical feasibility for attaining selected PM standards Umweltbundesamt Vienna, 23 February 2013

5 Service Request 6 final report Content 4.6 Detailed assessment of possible new standards, conclusions and recommendations DEVELOPING FUTURE OBJECTIVES FOR HEAVY METALS AND PAHS Key messages Context Extent of exceedances for heavy metals Current target values of the 4 th Daughter Directive Extent of exceedances of arsenic Extent of exceedances of cadmium Extent of exceedances of nickel Extent of exceedances of benzo(a)pyrene Assessment of industrial facilities and related monitoring sites Sources of exceedances Sources causing exceedances of target values for heavy metals Sources causing exceedances of the target value for B(a)P Necessary emission reductions Technical feasibility of emission reductions Cost of emission reduction Impact on health and environment of changes to current standards of As, Cd, Ni and B(a)P Thresholds for Hg Introduction Emissions, concentrations and deposition of Hg Action to reduce Hg emissions Possible thresholds for Hg Deposition of Heavy Metals and PAHs Quality of data Analysis of possible regulations INFORMATION OF THE PUBLIC UNDER THE 4 TH DAUGHTER DIRECTIVE Key messages Context requirements for information of the public Compiling reports and websites Reporting requirements under the Implementing Decision 2011/850/EC REFERENCES ABBREVIATIONS Umweltbundesamt Vienna, 23 February

6

7 Service Request 6 final report Summary SUMMARY The Air Quality Directive (AQD) and the 4 th Daughter Directive (DD4) to the Framework Directive both require a review of their provisions for PM 2.5 and arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons (PAH), respectively. The European Commission set up a service contract covering support in the review of these provisions. This report summarizes the work under this contract. It takes into account discussions that took place at two meeting with the European Commission, the PM workshop, which was held in Brussels in April 2012, the Stakeholder Expert Group meetings and first resulfts by WHO and IIASA. The services described in this contract include: Assessment of the current air quality situation for PM 2.5, PM 10, arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons, Assessment of current measurement practices of these pollutants, Development of future objectives for these pollutants covered, Assessment of information of the public and reporting. Assessment of the current air quality situation for PM 2.5, PM 10, arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons The analysis reported here was based on officially available datasets for PM 10, PM 2.5, As, Cd, Ni, Hg and PAH (B(a)P) concentration and deposition levels as well as emissions. Other pollutant specific issues, such as PM less than PM 2.5, were investigated. Finally, any significant data gaps were listed. The aim of presenting these data is to gain an overview of how levels vary across the entire area of Europe and to understand what conclusions can be drawn for each pollutant based on the weight of evidence from the different data sources. The analysis has shown that the PM 2.5 target value is only likely to drive action in a small number of Member States (MS). The Exposure Concentration Obligation may drive action in around eight MS. The National Exposure Reduction Target (NERT) may be challenging for many MS. There are many issues in trying to assess Average Exposure Indicator (AEI) from data available at the moment. In addition, there may be problems in calculating robust AEIs for 2010 (and therefore setting reliable NERT for MS) and in reliably measuring NERT over the 10 year period. According to the responses to the MS Questionnaire, no countries measured all of the chemical species listed in the AQD for characterising the chemical composition of PM 2.5. For nickel, cadmium and arsenic there are very few stations where exceedance of the target value is likely to drive action, as there are very few exceedances. There is more widespread exceedance of the target value for B(a)P than for the heavy metals. There are many exceedances in Poland and other Member States to the east of Europe. There are also more exceedances of the assessment thresholds than for the heavy metals. For nickel, arsenic and B(a)P the main data gap was a lack of projections data. This is a significant gap as it means that there is no available information on likely future changes. There are not many data available for mercury, either concentration or deposition. Further investigation may be needed into the reasons why so many MS have not provided total gaseous mercury data. Many MS have not reported any deposition data for nickel, cadmium, arsenic, mercury or B(a)P. The requirement and purpose of deposition measurements should be reviewed and either the Umweltbundesamt Vienna, 23 February

8 Service Request 6 final report Summary number of stations could be increased or it might be decided that deposition measurements are not needed at all. Assessment of current measurement practices of these pollutants A review of information on pollutant levels, their trends and data coverage is presented, including whether the data provided show inconsistencies which may be related to technical monitoring. Whether the datasets provided fulfil the basic requirements of the Directives (data capture, QA/QC) and whether there is any other monitoring undertaken by the Member States that is not submitted to the Data Exchange Module of EIONET (DEM) is presented. The main issues related to meeting the data quality objectives are listed and suggestions for improvement are made. The reported monitoring stations are compared to macroscale siting criteria. Even though the structure of the monitoring networks is quite heterogeneous the criteria are largely fulfilled. However, the number of PM 2.5 monitoring sites does not yet fulfil the requirements of the AQD. Also, MS rarely share rural background monitoring sites. The strengths, weaknesses and relevance of reference methods for PM 2.5 and PM 10 are discussed. These methods are not based on well defined measurands but on convention, and even thoroughly standardized still comprise considerable variability in results. Unfortunately this is also the case for all continuous methods (Automated Measurement Systems AMS) currently available. Procedures for equivalence demonstration of AMS may vary substantially between Member States. Currently, a new standard is being developed by the European Committee for Standardization (CEN) aiming at further normalization of equivalence procedures, taking into account spatial and temporal variability. Relationships between and specific issues of PM, heavy metals and PAH s are analysed, as is the suitability of B(a)P as a marker for the International Agency for Research on Cancer (IARC) 1 Probable and Possible Carcinogenic PAHs. The state of play in PM fractions is summarised, taking into account health effects, feasibility and the strength and weaknesses of monitoring techniques. Whether there is a need for new reference methods is discussed. Specific information on the practical aspects of measurement of organic carbon, elemental carbon, inorganic carbon, black carbon, anions and cations are summarised. However, other aspects such as relevance from a health effects point of view or the further development of monitoring techniques play an important role. Better understanding and definition of Black Carbon (BC) is needed. The measurement of BC is potentially a very useful tool, for health, traffic related pollutant indicator, high-level source apportionment (such as OC or UV carbon as a marker for biomass rather than fossil fuel combustion) and climate change issues. Benzo(a)pyrene, is still the only PAH with sufficient evidence to warrant classification as a human carcinogen. It has been used as a surrogate for all the other PAH, although there is insufficient evidence to say that it is not still valid as the marker. The additional PAH selected for assessment within DD4 cover most, but not all, of the PAH in the IARC list and miss some additional PAH that can help with source apportionment studies. While some MS will measure a wider range of PAH, this is not guaranteed Umweltbundesamt Vienna, 23 February 2013

9 Service Request 6 final report Summary Development of future objectives for PM The AQD has set standards for particulate matter (PM) in ambient air and requires the Commission to review the PM 2.5 standards. The study described in this report supports this review by exploring possibilities for updating and improving the standards. This assessment also includes considerations about other PM metrics such as PM 10, ultrafine particles (UFP), Black Carbon (BC) and further constituents of PM. The study started with an inventory of the current state of implementation of the provisions relating to the PM 2.5 standards regarding assessment and management. It included data reported under the directive to the Commission and other information such as consultations of stakeholders in questionnaires, a workshop on PM and experience from the US in managing PM 2.5. Most measures for PM 10 and NO 2 reduce PM 2.5 levels as well with the exemption of few measures that address mechanical generated dust. Measures to reduce emissions of precursors support the reduction of PM 2.5 levels. Important input to the investigation was the first results of the recent evaluation by WHO of the health impacts of PM (WHO 2013). The study aimed to identify possibilities for changing properties of the PM standards and to systematically assess the added value of such changes. To this end a set of evaluation criteria was drawn up. All properties of the standards were considered: the PM fraction regulated, the binding nature, the level to be attained, the attainment year, other temporal aspects and spatial aspects. The suitability of possible changes was analysed and where possible conclusions were drawn. However it is difficult to objectively balance advantages and drawbacks, which are often different in nature. Nevertheless, the analysis that has been compiled provides useful rationale for the review process. Reduction of PM is likely to be effective for reducing the health impact at all concentration levels found in the EU. To avoid that a fully binding level to be attained everywhere will only drive down levels at the most unfavourable locations, we recommend considering lower, more ambitious levels in combination with flexibility provisions for locations where the standard cannot be met (derogations such as the current time extension provisions, spatial differentiation to exclude certain areas with persistent problems). We therefore also recommend strengthening the binding nature of the National Exposure Reduction Target for PM 2.5. Recommendations on the numerical level of the PM standards are not given in this report; they should be based on detailed analysis of model projections taking into account the most recent information. Several refinements of more technical possibilities were investigated such as a possible threeyear compliance period for the limit values, a reduced averaging area of the Average Exposure Indicator. Options for new standards were also considered, in particular a 24-hour limit value for PM 2.5 and standards for black or elemental carbon and for ultrafine particulates. WHO has stressed the importance of all existing PM standards, but in view of the desire of Member States and other stakeholders to use the partial overlap of the standard for simplifying the set of PM standards, possibilities were explored for withdrawing possibly redundant standards without decreasing the overall protection provided by the PM standards. Umweltbundesamt Vienna, 23 February

10 Service Request 6 final report Summary Assessment of objectives for heavy metals The analysis of heavy metal concentrations has shown that reported exceedances of the existing target values are associated with a small number of industrial sources. There is some evidence that the existing target values are ensuring that measures are being taken to tackle these industrial exceedances by reducing emissions. However, detailed understanding of the relationships between sources and ambient concentrations is scarce. Also information is missing on the assessment and concentration levels around several sources that emit high quantities of heavy metals. For those sources where exceedances have been reported only in very few cases detailed information on the impact and costs of measures is available. More information on measures and their impact may become available once the existing target values come into force in 2013 and mandatory reporting by Member States on measures commences. Assessment of objectives for benzo(a)pyrene Exceedances of the target value for benzo(a)pyrene as a representative for PAH occur in several Member States and affect several million people. Most of the reporting exceedances are associated with domestic heating emissions; some are caused by industrial emissions. However, there is very little quantitative evidence available of the impact of the abatement measures that have been and will be taken. A reduction of the target value to a much lower level would result in widespread exceedances across almost all of the EU. Assessment of possible objectives for mercury Measurement of mercury concentration in ambient air is scarce; the levels observed are in the order of magnitudes below guideline values for ambient air. Exposure to ambient air concentrations is not a significant contributor to human exposure to mercury, which is mainly driven by dietary exposure and dental amalgam. Therefore it is recommended continuing of monitoring ambient concentrations of Hg in both urban areas and industrial hotspots and continuing abatement of emissions on international level. An implementation of a target value for mercury would not result in a significant reduction of exposure to mercury. Deposition of heavy metals and PAH There is few deposition data available for heavy metals and PAH collected with the reference measurement methods. Available data show a wide range between industrial sites and background sites; so a different sampling strategy is needed for these two different types of sites. As there is a considerable influence in the use of different collector types to measured deposition rates, it is recommended to gain more information on and experience with the current reference measurements methods before setting target or limit values by additional deposition monitoring on background and industrial sites. Assessment of information of the public and reporting under DD4 To assess the information of the public and the reporting under DD4 the availability of the required information made available by the Member States via internet has been investigated. The analysis has shown that the pollutants regulated by DD4 are published in annual reports. The access to these reports is usually quite easy and straightforward. About two third of the Member States comply fully with the requirements for information of the public, six Member States either do not publish heavy metal and PAH data or do not monitor these pollutants. 10 Umweltbundesamt Vienna, 23 February 2013

11 Service Request 6 final report Summary Within this study also possible changes for reporting due to the Commission Implementing Decision laying down rules for Directives 2004/107/EC and 2008/50/EC of the European Parliament and of the Council as regards the reciprocal exchange of information and reporting on ambient air quality 2011/850/EU were analysed. It is shown that this decision doesn t change the present reporting requirements for the pollutants regulated by the DD4. Umweltbundesamt Vienna, 23 February

12

13 Service Request 6 final report Introduction 1 INTRODUCTION According to Article 32 of Directive 2008/50/EC on ambient air quality and cleaner air for Europe ( Air Quality Directive, AQD), the Directive s provisions related to PM 2.5 and, as appropriate, other pollutants shall be reviewed in In addition, a review is foreseen according to Article 8 of Directive 2004/107/EC relating to arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons in ambient air ( 4 th Daughter Directive, DD4). The European Commission set up a service contract with Umweltbundesamt, Ricardo AEA and TNO covering support in the review of the provisions related to PM 2.5 and PM 10 in the AQD as well as the provisions related to all pollutants covered by the DD4 (specific contract number /2011/599749/SER/C3). The contract came into force on 10 August 2011 and has a duration of 16 months. The services described in this contract include: Assessment of the current air quality situation, Assessment of current measurement practices, Development of future objectives for the pollutants covered by the review, Assessment of information of the public and reporting. To provide these services, the work is divided into seven tasks: Task 1: Assessment of current air quality situations, projections and reduction potentials in the Member States (chapter 2). Task 2: Review of assessment methodologies for РM 10, PM 2.5, heavy metals and PAHs with particular emphasis on measurement practices (chapter 3). Task 3: Developing future objective(s) for PM 2.5 (chapter 4). Task 4: Developing future objectives for heavy metals and PAHs (chapter 5). Task 5: Addressing other aspects in the review of the 4 th Daughter Directive (chapter 6). Task 6: Consultation and updating of results (the results of this task are summarized in meeting reports and further documentation). Task 7: Meetings, preparation and follow-up (the results of this task are summarized in meeting reports). This final report is based on the specific reports for Task 1 to 5 (RICARDO AEA 2012; RICARDO AEA, UMWELTBUNDESAMT & TNO 2012; TNO, UMWELTBUNDESAMT & RICARDO AEA 2013; UMWELTBUNDESAMT & RICARDO AEA 2012; UMWELTBUNDESAMT 2012). Umweltbundesamt Vienna, 23 February

14 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials 2 ASSESSMENT OF CURRENT AQ SITUATIONS, PROJECTIONS, REDUCTION POTENTIALS 2.1 Key messages PM 10 In just over half of all MS all monitoring stations were in compliance with the PM 10 annual limit value in Most of the exceeding monitoring stations are in Eastern Europe or Italy. Almost all MS had a least one monitoring station in exceedance of the PM 10 daily limit value in The main data gap in the work on PM 10 was that no data were available on PM 10 concentrations in These data were not in the 2010 questionnaires 2004/461/EC and the updated version of AirBase that included 2010 data was not available during the timescale of Task 1 (summarized in this chapter) of this project. PM 2.5 The PM 2.5 target value is only likely to drive action in a small number of MS. The Exposure Concentration Obligation (ECO) may drive action in around eight MS. The National Exposure Reduction Target (NERT) may be challenging to many MS, especially those with highest current concentrations. There are many issues in trying to assess AEI from data available at the moment. The Commission should scrutinise the 2011 Questionnaire 2004/461/EC in great detail for Average Exposure Indicator (AEI) and it is likely that direct engagement with the MS will be needed. The compliance statistics for PM 10 and PM 2.5 presented in the current report (including AEI and ECO) should help to inform the review as to which limits are more likely to drive action. There may be problems in calculating robust AEIs for 2010 and therefore setting reliable NERT for MS. In addition, there may be a potential problem in reliably measuring NERT over the 10 year period. AQUILA have published draft guidance on calculating the AEI (AQUILA 2012). However, there is further work to do on the AEI and other bodies and projects such as AQUILA are likely to be involved in further looking in to these issues. PM less than PM 2.5 According to the responses to the MS Questionnaire, no countries measured all of the species listed in the AQD for characterising the chemical composition of PM 2.5. Seven countries measured only one of the species and four countries measured between four and six. The reason for the lack of data on PM less than PM 2.5 should be investigated. Possibly additional monitoring of PM 1 or black carbon (for example) should be mandatory in new AQD. However, it should be considered how this could be done without placing a large burden on MS and without a specific environmental objective being set. Nickel There are very few stations where exceedances of the target value is likely to drive action, as there are very few exceedances. The stations that are in exceedance are mostly industrial 14 Umweltbundesamt Vienna, 23 February 2013

15 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials stations (though one is a traffic station). In addition, there are only a small number of stations with concentrations greater than the assessment thresholds for nickel. Many MS have not reported any nickel deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. The main data gap was a lack of projections data. This is a significant gap as it means that there is no available information on likely future changes. Cadmium There are very few stations where exceedance of the target value is likely to drive action, as there are very few exceedances. The exceedances are mostly at industrial stations, but there are also exceedances at two background and one traffic station. There are also only a small number of stations with concentrations greater than the assessment thresholds for cadmium. Many MS have not reported any cadmium deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. Arsenic There are very few stations where exceedance of the target value is likely to drive action, as there are very few exceedances. The exceeding stations are mostly industrial, but there are also four exceedances at background stations. However, there are more stations with concentrations greater than the assessment thresholds for arsenic than for nickel and cadmium. Many MS have not reported any arsenic deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. The main data gap was a lack of projections data. This is a significant gap as it means that there is no available information on likely future changes. B(a)P There is more widespread exceedance of the target value for B(a)P than for the heavy metals. There are many exceedances in Poland and other Member States to the east of Europe. There are exceedances of the target value at some industrial stations and traffic stations but most of the exceedances are at background stations. The use of solid fuel for domestic heating is likely to be the main source associated with the exceedances. There are also more exceedances of the assessment thresholds than for the heavy metals. Many MS have not reported any B(a)P deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. The main data gap was a lack of projections data. This is a significant gap as it means that there is no available information on likely future changes. Umweltbundesamt Vienna, 23 February

16 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Mercury There are not many data available for mercury; not many MS have provided total gaseous mercury data in the 2010 Questionnaire 2004/461/EC. Further investigation may be needed into the reasons why so many MS have not provided total gaseous mercury data. Many MS have not reported any mercury deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. Reduction potentials Data reported by MS in the Questionnaire 2004/461/EC and emissions data did not necessarily indicate that the same sources are important. In addition, national emissions can only provide an indication of possible sources. As the exceedances may be confined to small areas, on a local level further sources might be of relevance, which might not show a large contribution to emissions on a national scale. Task 4 (section 5) will provide more detail on sources. The major data gap in completing the assessment of reduction potential was the lack of recent source apportionment data for heavy metals and B(a)P. 2.2 Introduction Basis The basis of this assessment are the two Directives, Directive 2008/50/EC of the European Parliament and of the Council of 21 May 2008 on ambient air quality and cleaner air for Europe, this can be referred to as the Air Quality Directive (AQD) and Directive 2004/107/EC of the European Parliament and of the Council of 15 December 2004 relating to arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons in ambient air, which can be referred to as the Fourth Daughter Directive (DD4). Specifically a review is required of the following topics: Article 32 of AQD requires a review of the regulations for PM 2.5 and, as appropriate, other pollutants, Art 32.3 provides for the necessity to prepare a report of the experience of monitoring PM 10 and PM 2.5. Article 8 of DD4 requires a report about the implementation of the directive and a review of the targets for arsenic (As), cadmium (Cd), nickel (Ni), mercury (Hg) and polycyclic aromatic hydrocarbons (PAH). This report forms part of the review under the provisions listed above. The environmental objectives from these Directives pertinent to this report are given in Summary Table 1, with the exception of Hg, which does not have a prescribed target or limit value. 16 Umweltbundesamt Vienna, 23 February 2013

17 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Table 1: Environmental Objectives of the Air Quality Directive and the 4 th Daughter Directive. Determinant Limit Type Short Name Description PM 10 Limit Annual LV A calendar year average concentration of 40 µg/m³ PM 2.5 National Exposure Reduction Target Daily LV NERT A daily concentration of 50 µg/m³ not to be exceeded more than 35 times in one calendar year A comparison of the three year mean (AEI) up to 2020 to the three year mean 2008 to 2010 where the future three year mean value is either less than 8.5 µg/m³ or other reduction target based on the initial concentration Target TV A calendar year average concentration of 25 µg/m³ Exposure concentration obligation ECO 20 µg/m³ (applies to the AEI) in 2015 As Target TV 6 ng/m³ for the total content in the PM 10fraction averaged over a calendar year Cd Target TV 5 ng/m³ for the total content in the PM 10fraction averaged over a calendar year Ni Target TV 20 ng/m³ for the total content in the PM 10fraction averaged over a calendar year Benzo(a)Pyrene (B(a)P) Target TV 1 ng/m³ for the total content in the PM 10fraction averaged over a calendar year - B(a)P is a specific type of PAH that has been adopted within the framework of DD4 as representative of the fate and behaviour of the other PAH. The National Emissions Ceilings Directive (NECD) is not the focus of this report so, none of the pollutants covered in NECD are directly assessed but emissions of those pertinent to PM precursors are provided alongside the sector type emissions data for the PM fractions that are the focus of this report Data sources AirBase and the annual Questionnaire For historical and current data, two datasets were used, AirBase 2 and the Questionnaire according to Decision 2004/461/EC (in the following referred to as questionnaire 2004/461/EC ). This assessment uses available data in AirBase for for the analysis of the ambient concentrations in the years for all pollutants. The level of meta-data associated with the concentration and exceedance statistics is reasonable for the AirBase data. As the AirBase data for 2010 were not available on the timescale of Task 1 of this work, the data from completed Member State (MS) annual assessment questionnaires 2004/461/EC for 2010 were used for all pollutants except PM 10 for which only AirBase data were used (the year 2010 was not included in the analysis for this pollutant). This is because for PM 10 only exceedances are reported in the Questionnaire and therefore annual average concentrations for all stations were not available for The most recent available data for PM 10 were the 2009 data from AirBase. 2 Umweltbundesamt Vienna, 23 February

18 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials The Questionnaire 2004/461/EC data submitted by each MS contains a number of inconsistencies, namely: Concentration and deposition rates stored as text rather than as a number. Deposition data given in different units to that requested. Pollutants given in a different order to that requested. Additional descriptions given, leading to a wide gulf between the prior data to 2009 reported in AirBase and that reported in the Questionnaires. Lack of data capture statistics in the Questionnaire. The data have been taken at face value, with the assumption that the MS has made every endeavour to ensure that the data presented are, as far as can be reasonably expected, a true estimate of the concentration and deposition rates. A data capture threshold of 90 % has been applied to the AirBase data, in line with required proportion of valid data of Annex XI of the AQD. Where the data capture was reported in the Questionnaire data this information was used and a 90 % data capture threshold was also applied, however in general no data capture information was given, so 90 % data capture was assumed Emissions data The historic trends in emission have been included for the years 2000 to These data have been taken from the UNECE/EMEP Centre on Emission Inventories and Projections (CEIP 3 ) emissions database (WebDab 4 ). The data are reviewed annually. The emissions used in the EMEP models data were downloaded for each MS (and Croatia), the data for PM 10 and PM 2.5 were resolved by SNAP code. The emissions used in the EMEP models data for the DD4 pollutants is held as MS emission totals only. The SNAP sector totals of the officially reported emissions have been used for assessing the reduction potential of heavy metals and B(a)P. For assessing the reduction potential of heavy metals (chapter 2.11), data from the ESPREME 5 project were also used. The project included calculating emissions and concentrations projections for 2000 to 2010 for heavy metals (arsenic, cadmium, chromium, mercury, nickel and lead) disaggregated by sector. There are large differences between these datasets for some MS and for some pollutants, so these data have not been presented together. For most MS and pollutants the total from the ESPREME project is larger than the total from WebDab, but this is not always the case (see Table 9.3 of the task 1 report, RICARDO AEA 2012) Projection data The CCE Status report 2010 studied emissions and concentrations projections of cadmium, mercury and lead and these concentrations projections are presented in this report (CCE 2010). For the projections data presented in this report three of the scenarios from this report were used: CLE2010, which is the current legislation projection for 2010 from a base year of FI20, which is a projection for 2020 that includes full implementation of the HM protocol in all UNECE Europe MS Umweltbundesamt Vienna, 23 February 2013

19 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials FI20_op1, which includes the possible revision of the HM protocol due to the implementation of measures outlined in the Draft possible amendments to the 1998 HM Protocol (UNECE 2009). It includes the most stringent emission limit values for major stationary sources in Annex V.II of the 1998 protocol. Recent data on projections of ambient concentrations of arsenic, nickel and benzo(a)pyrene are not available Member State Questionnaire A questionnaire was circulated to MS in February 2012 in order to request further information that was not available from other data sources (such as the Questionnaire 2004/461/EC) in order to assess the current scale and quality of monitoring measurements across MS (including information on the AEI and measurements of PM less than PM 2.5 ) Comparison of monitoring data with limit values, target values and assessment thresholds The level of rounding of monitoring data that should be done before comparison with the limit values, target values and assessment threshold is currently unclear. It appears from the 2010 Questionnaires 2004/461/EC that different MS have used different levels of rounding in their officially reported values. In order to use a consistent approach throughout this report, all measured data are rounded to 1 decimal place before comparing with the limit values, target values and assessment thresholds. Therefore the exceedance numbers presented in this report might be different to the officially reported data in some cases. The Commission has clarified that the AEI should be rounded to 1 decimal place and also the initial AEI concentration threshold should be rounded to 1 decimal place as well. Clarification on the level of rounding required for the target values of DD4 is foreseen for the review of the AQD and a consistent approach from all MS should be the case in the future Report Structure The work presented here seeks to contribute to the review through an analysis of officially available datasets for PM 10, PM 2.5, As, Cd, Ni, Hg and PAH (B(a)P). Specific attention is given to: Ambient concentration measured and reported by MS (current and historical levels) focused on and limited to, metrics for which environmental objectives have been set within the Directives. Where no environmental objectives exist, the annual average concentrations have been considered. Data for the years up to and including 2009 have been used for the PM 10 analysis and data for the years up to and including 2010 have been used for the analysis for all other pollutants. Annual Emission trends for MS up to and including Deposition rates reported by MS for relevant pollutants. Other pollutant specific issues. The analysis is presented by pollutant, as this will provide a better synthesis of what the different data sources show for each. Geographically, this report covers the reported data from the EU27 MS and Croatia, collectively referred to as the MS. Umweltbundesamt Vienna, 23 February

20 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials The data are presented with the dual aims: To gain an overview of how levels vary across the entire area of Europe covered by this review. To understand what conclusions can be drawn for each MS for each pollutant based on the weight of evidence from the different data sources. The focus of the analysis in this report will be at MS level. New analysis by EU reporting zone will not be carried out since this type of analysis is routinely reported by the EEA. However, for completeness, we will present a summary of the EEA findings where relevant. An additional section is provided that addresses the relationship between the DD4 pollutants measured and the relevant PM fraction in which these have been measured Work covered by this task Table 2 provides a master summary of the topics to be covered for each of the pollutants to be considered. Table 2: Checklist of work covered by this task. Topic PM 10 PM 2.5 PM below PM 2.5 As, Cd, Ni, B(a)P Hg NO 2 Ambient concentrations: a snapshot of current levels Ambient concentrations: Historic trends Ambient concentrations: Projections Emissions: Historic trends Emissions: Projections Average Exposure Indicator PM below PM 2.5 Deposition Reduction potential for Member States Specific dataset: Summary statistics for IIASA Specific dataset: Population exposure 2.3 PM 10 Three groups of analysis have been carried out for PM 10 : Analysis of current (2009) ambient PM 10 annual mean concentrations and daily exceedance statistics. Analysis of historic trends in ambient PM 10 concentrations. 20 Umweltbundesamt Vienna, 23 February 2013

21 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Analysis of historic trends in emission of PM 10. It should be noted that projections of PM 10 have not been considered as part of this work. In addition to the data presented here, summary statistics from AirBase for PM 10 and PM 2.5 in 2009 were also provided to IIASA. These data were provided for priority stations only. Priority stations were those with exceedances of PM 10 annual or daily limit values in 2009, exceedances of PM 2.5 target value in 2009 or those stations that were listed as AEI stations in the 2009 questionnaire. The annual mean limit value and upper/lower assessment thresholds given in the AQD for PM 10 are: Limit value: 40 µg/m³ in a calendar year. Upper assessment threshold: 28 µg/m³. Lower assessment threshold: 20 µg/m³. In just over half of all MS all monitoring stations were in compliance with the PM 10 annual limit value in The largest compliance gap was 42.6 µg/m³ at a traffic station in Italy. Most of the exceeding monitoring stations are in Eastern Europe or Italy. Bulgaria was the only MS with an average concentration for PM 10 above the limit value at 46.8 µg/m³, from a total of 37 stations reported. Almost all MS had a least one monitoring station in exceedance of the PM 10 daily limit value in The largest compliance gap was 254 exceedances at a traffic station in Italy. Almost all MS have had at least one exceedance between 2001 and For most MS these exceedances are across the station types, but roadside stations sometimes dominate. Only thirteen MS have a time series of PM 10 monitoring data longer than seven years. For Germany, Belgium and Austria there is a statistically significant downward trend in PM 10 concentrations between 2000 and For France there is a statistically significant upward trend (but is likely to be due to a change in monitoring method). The measurement method used to gather the French PM 10 data was predominantly using TEOMs and the French authorities changed the correction method in For the other MS there is no statistically significant trend. The primary PM 10 emissions decreased between 2000 and 2009 for almost all MS. For most MS there is a decline in concentrations that is reasonably consistent with the decline in primary emissions. However it is recognised that part of the trend in measured concentrations will be associated with the trends in secondary PM, for which the precursor emissions of SO 2 and NO x also show declines in many MS. The main data gap in the work on PM 10 was that no data were available on PM 10 concentrations in These data were not in the 2010 questionnaires 2004/461/EC and the updated version of AirBase that included 2010 data was not available during the timescale of Task 1 this project. For most MS the trends in PM 10 and PM 2.5 concentrations are broadly consistent, though there are generally less data available for PM 2.5 than PM PM 2.5 Four groups of analysis have been carried out for PM 2.5 : Analysis of current (2010) ambient PM 2.5 annual mean concentrations Analysis of historic trends in ambient PM 2.5 concentrations Umweltbundesamt Vienna, 23 February

22 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Analysis of historic trends in emission of PM 2.5. The calculation and assessment of the Average Exposure Indicator (AEI). No PM 2.5 projections have been included in this data analysis task. A projection prepared by IIASA for the review is available. In addition to the data presented here, summary statistics from AirBase for PM 10 and PM 2.5 in 2009 were also provided to IIASA. These data were provided for priority stations only. Priority stations were those with exceedances of PM 10 annual or daily limit values in 2009, exceedances of PM 2.5 target value in 2009 or those stations that were listed as AEI stations in the 2009 Questionnaire 2004/461/EC. The annual mean target value and upper/lower assessment thresholds for PM 2.5 are: Target value: 25 µg/m³. Upper assessment threshold: 10 µg/m³. Lower assessment threshold: 7 µg/m³ Analysis of current (2010) ambient PM 2.5 annual mean concentrations In 2010, many monitoring stations in most MS were below the PM 2.5 target value. However, there were exceeding monitoring stations in Germany, France, Italy, Poland, Czech Republic, Hungary, Bulgaria, Slovakia and Latvia. The majority of exceedances were at background stations. The largest compliance gap in 2010 was 36 µg/m³ at a traffic station in Poland (Figure 1). Figure 1: Annual mean PM 2.5 levels in 2010 (in µg/m³. Minimum, 10 th percentile, mean, 90 th percentile, maximum levels and target value. Source: 2010 Questionnaire 2004/461/EC). Just over half of the MS have had at least one monitoring station exceeding the PM 2.5 target value between 2001 and However, many of those exceedances are only exceeding the target value by a small amount Analysis of historic trends in ambient PM 2.5 concentrations Only thirteen MS have a time series longer than five years. For Italy there is a statistically significant downward trend in PM 2.5 concentrations at background stations only between 2001 and For Portugal there is a statistically significant downward trend over the same time period for industrial stations only. For Hungary and Sweden there is a statistically significant downward 22 Umweltbundesamt Vienna, 23 February 2013

23 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials for traffic stations only. There are no statistically significant upward trends for PM 2.5 concentrations (for those MS that have a time series longer than 5 years). For the other MS there is no statistically significant trend. There are not enough data available to find an overall picture in trends. The German dataset is shown as an example (Figure 2). Figure 2: Annual mean PM 2.5 concentration trends for Germany (in µg/m³, Source: AirBase) Analysis of historic trends in emission of PM 2.5 There is a decrease in primary PM 2.5 emissions for most MS between 2000 and 2010 (Figure 3). For those 22 MS for which emission data is available since 2000, the overall emissions decreased by 16 % from 2000 to An increase was reported for BG, DK, EE, FI, LV, PL, SI and SE. Umweltbundesamt Vienna, 23 February

24 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials PM2.5 emissions in kt RO CZ SE SI PT NL LV IE DE FI DK BG AT LT UK ES SL PL MT IT HU FR EE CY BE Figure 3: PM 2.5 emissions in EU MS 2000 to 2010 (officially reported data. Source: CEIP) Calculation and assessment of the Average Exposure Indicator (AEI) Indicative AEIs were calculated for 2010 using 2010 Questionnaire according to Decision 2004/461/EC data, 2009 Questionnaire according to Decision 2004/461/EC data and 2009 Air- Base data. Five MS have best estimate AEIs above 22 µg/m³ and therefore their indicative Exposure Reduction Target (ERT) would be to take all appropriate measures to achieve 18 µg/m³. Most MS have best estimate AEI of between 13 µg/m³ and 18 µg/m³ and therefore have an indicative ERT of 15 % (see Table 3.6 of Task 1 report for details, RICARDO AEA 2012). Eight MS (Bulgaria, Cyprus, Czech Republic, Hungary, Italy, Poland, Slovakia and Slovenia) have best estimate AEIs for 2010 that are above the Exposure Concentration Obligation (20 µg/m³), which will be legally binding in There is a lack of data related to the AEI reported in the 2010 Questionnaire 2004/461/EC. However, these gaps were expected to be filled in the 2011 Questionnaire 2004/461/EC, when all MS should have reported their final AEI 2010 values. Many MS reported a final AEI 2010 value in the 2011 Questionnaire 2004/461/EC, but there were still missing data. In addition within this project a specific questionnaire was sent to MS on 11 September 2012, where the PM 2.5 exposure reduction obligation was requested. The information received from MS is described in Task 3 (see specific report, TNO, UMWELTBUNDESAMT, RICARDO AEA 2013, summarized in section 4). In addition, the MS highlighted issues with data capture, the moving of monitoring stations and general issues related to measurement of PM 2.5 in their responses to our previous questionnaire, which was sent out in February They also highlighted the requirement for clear guidance on the methods that should be used to calculate the AEI. It is important that a specific method of calculation is defined, including whether a data capture threshold should be used (and if so what it should be) and guidance on whether all stations should be included or whether there needs to be a minimum number of valid years for the station to be included. Some guidance on this can be found in the IPR (Decision 2011/850/EU). The method of calculation of the AEI has been considered by AQUILA and recommendations 24 Umweltbundesamt Vienna, 23 February 2013

25 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials for the methodology for defining the requirements that stations that are used to monitor PM 2.5 concentrations, in order to provide data that the AEI and its associated parameters, should conform to, including proposals for (AQUILA 2012): Selection of the monitoring stations, as far as practical; Procedure(s) for calculating the required annual averages from the individual daily or integrated-hourly measured PM 2.5 data at the selected monitoring stations; Methods for averaging the annual datasets from the selected stations to produce the average annual values from all the monitoring stations; Determination of the Average Exposure Indicator (AEI) for a Member State by averaging all the valid annual results at all the specified locations. A recommendation that the procedure for forming the three-year averaged AEI by weighting the concentrations from the selected measurement stations with their data capture should be applied to all the AEI calculations - that is: The AEI for the initial reference year AEI that is then used to define the NERT, The AEI in years necessary for an examination of whether the ECO is met, The AEI in years necessary to determine whether the NERT is achieved, and the AEIs that are to be reported for all other three year periods that are required (see specific report for Task 2 for further details, RICARDO AEA, UMWELTBUNDESAMT & TNO 2012, summarized in section 3). Uncertainties in the measurements and within the calculation of delta AEI may mean that it is not possible to assess the delta AEI against the ERT. New analysers, service and maintenance, variability in analyser performance and changes to the Reference Method could mean that the uncertainty of measuring the delta AEI could be greater than that needed to robustly assess a required reduction of 2.0 µg/m³ in PM 2.5 concentrations between 2010 and However different groups have reached different conclusions on this (RICARDO AEA 2011, MATTHIJSEN et. al. 2009). Further investigation is needed on whether the delta AEI can be calculated with enough confidence to assess it against the ERT. AQUILA has published guidance for improving the consistency of the AEI between 2010 and 2020 (AQUILA 2012). For most MS the trends in PM 10 and PM 2.5 concentrations are broadly consistent, though there are generally less data available for PM 2.5 than PM 10. There are only limited data available for PM 2.5 (see also section 2.4.2). The PM 2.5 target value is only likely to drive action in a small number of MS. The ECO may drive action in around eight MS. The NERT may be challenging to many MS, especially those with highest current concentrations. There are many issues in trying to assess AEI from data available at the moment. The Commission should scrutinise the 2011 Questionnaire 2004/461/EC in great detail for AEI and it is likely that direct engagement with the MS will be needed. Some additional data and information is available from the replies to the specific questionnaire sent out in September The compliance statistics for PM 10 and PM 2.5 presented in this section (including AEI and ECO) should help to inform the review as to which limits are more likely to drive action (RICARDO AEA 2012). There is further work to do on the AEI and other bodies and projects such as AQUILA are likely to be involved in further looking in to these issues. Umweltbundesamt Vienna, 23 February

26 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials 2.5 PM below PM 2.5 and constituents The AQD states that the list of chemical species given below shall be included in the measurement of concentrations of appropriate compounds to characterise the chemical composition of PM 2.5 : SO 4 2 NO 3 Na 2+ K + NH 4 + Cl Ca 2+ Mg 2+ elemental carbon (EC) organic carbon (OC) Seven countries did not respond to the MS Questionnaire (Bulgaria, Croatia, Finland, Hungary, Malta, Portugal and Slovakia). Cyprus, Greece, Lithuania, Luxemburg, Romania and Slovenia reported only one of these species were measured. No countries measured all of the species, the Czech Republic, France, Poland, Spain and the UK measured between four and six. The reason for the lack of data on PM less than PM 2.5 should be investigated. Possibly additional monitoring of PM 1 or black carbon (for example) should be mandatory in new AQD. However, it should be considered how this could be done without placing a large burden on MSs and without a specific environmental objective being set. 2.6 Nickel Seven groups of analysis have been carried out for nickel: Analysis of current (2010) levels of nickel annual mean concentrations. Analysis of historic trends in ambient nickel. Ambient concentration projections. Analysis of historic trends in emissions of nickel. Emission projections. Deposition of nickel. Reduction potential of MS for nickel. The annual mean target value and upper/lower assessment thresholds for Ni are: Target value: 20 ng/m³. Upper assessment threshold: 14 ng/m³. Lower assessment threshold: 10 ng/m³. In 2010 all monitoring stations were below the nickel target value in most MS. A few stations in Germany, Spain and Belgium were in exceedance. The largest compliance gap was 48.5 ng/m³ at an industrial station in Germany. 26 Umweltbundesamt Vienna, 23 February 2013

27 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials The vast majority of MS have no measured exceedances of the nickel target value between 2001 and Only Germany, France, United Kingdom, Italy, Spain and Belgium had measured exceedances during this period. There were insufficient data for trend analysis on the ambient trends between 2001 and 2010 (due to a lack of data for the earlier years). MS emissions of nickel decrease between 2000 and 2009 for all MS with data available except three (Czech Republic, Croatia and Cyprus). The trends in nickel emissions are reasonably consistent with trends in PM 10 emissions for some MS. There are not enough data on nickel deposition available to draw any conclusions on deposition. There are a lot more data available in 2009 and 2010, than in previous years, but most of the additional data are from Germany. There were a few data gaps for nickel: No projections data (for emissions or concentrations). No modelled deposition data. Webdab emissions data are not available for all MS. The lack of projections data is a significant gap as it means that there is no available information on likely future changes. There are very few stations where exceedances of the target value is likely to drive action. The stations that are in exceedance are mostly industrial stations (though one is a traffic station). In addition, there are only a small number of stations with concentrations greater than the assessment thresholds for nickel. Many MS have not reported any nickel deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. 2.7 Cadmium Seven groups of analysis have been carried out for cadmium, being: Analysis of current (2010) levels of cadmium annual concentrations. Analysis of historic trends in ambient cadmium. Ambient concentration projections. Analysis of historic trends in emissions of cadmium. Emission projections. Deposition of cadmium. Reduction potential of MS for cadmium. The annual mean target value and upper/lower assessment thresholds for Cd are: Target value: 5 ng/m³. Upper assessment threshold: 3 ng/m³. Lower assessment threshold: 2 ng/m³. Umweltbundesamt Vienna, 23 February

28 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials All monitoring stations in most MS are below the cadmium target value in There were exceeding monitoring stations in France, Spain, Belgium, Bulgaria and Finland. The largest compliance gap was 20.4 ng/m³ at a background station in Bulgaria. Most MS did not have any exceeding monitoring stations between 2001 and 2010, though there are a large number of exceedances of the target value in Belgium in every year from 2001 to Many MS do not have a large amount of monitoring data for this period and there were insufficient data for trend analysis on the ambient trends between 2001 and 2010 (due to a lack of data for the earlier years). There is a decrease in cadmium emissions between 2000 and 2009 in just over half of the MS, with thirteen of these showing a steady reduction between the two years. However, there is a significant number of MS that show an increase in emissions during this period. According to the CCE Status Report 2010 data, cadmium concentrations are predicted to decrease between 2010 and 2020 for all MS (in the most ambitious scenario) (CCE 2010). However, for the least ambitious scenario emissions are only predicted to decrease for just over half of the MS and increase for just under half of the MS. There are not enough data on cadmium deposition available to draw any conclusions on deposition. There are a lot more data available in 2009 and 2010, than in previous years, but most of the additional data are from Germany. The problems and gaps encountered in the data are: Webdab emissions data are not available for all MS. There are very few stations where exceedance of the target value is likely to drive action. The exceedances are mostly at industrial stations, but there are also exceedances at two background and one traffic station. There are also only a small number of stations with concentrations greater than the assessment thresholds for cadmium. Many MS have not reported any cadmium deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. 2.8 Arsenic Seven groups of analysis have been carried out for arsenic, being: Analysis of current (2010) levels of arsenic annual concentrations. Analysis of historic trends in ambient arsenic. Ambient concentration projections. Analysis of historic trends in emissions of arsenic. Emission projections. Deposition of arsenic. Reduction potential of MS for arsenic. The annual mean target value and upper/lower assessment thresholds for arsenic are: Target value: 6 ng/m³. Upper assessment threshold: 3.6 ng/m³. 28 Umweltbundesamt Vienna, 23 February 2013

29 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Lower assessment threshold: 2.4 ng/m³. In 2010 most MS had no exceedances of the arsenic target value measured at any monitoring stations. However, exceedances were measured at some monitoring stations in Germany, Poland, Belgium, Czech Republic and Finland. The largest compliance gap was 38.2 ng/m³ at a Belgian industrial station. Like the other heavy metals, most MS have had all monitoring stations below the target value throughout the period between 2001 and However, there are a large number of exceedances of the target value in Belgium in every year from 2001 to For many MS there is a limited amount of data. There were insufficient data for trend analysis on the ambient trends between 2001 and 2010 (due to a lack of data for the earlier years). There is a decrease in arsenic emissions between 2000 and 2009 in the majority of the MS. However, there is a significant number of MS that show an increase in emissions during this period. There are not enough data on arsenic deposition available to draw any conclusions on deposition. There are a lot more data available in 2009 and 2010, than in previous years, but most of the additional data are from Germany. The problems and gaps encountered in the data are: No projections data (emissions and concentrations). No modelled deposition data. Webdab emissions data are not available for all MS. The lack of projections data is a significant gap as it means that there is no available information on likely future changes. There are very few stations where exceedance of the target value is likely to drive action. The exceeding stations are mostly industrial, but there are also four exceedances at background stations. However, there are more stations with concentrations greater than the assessment thresholds for arsenic than for nickel and cadmium. Many MS have not reported any arsenic deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all. 2.9 Benzo(a)pyrene Seven groups of analysis have been carried out for benzo(a)pyrene: Analysis of current (2010) levels of benzo(a)pyrene annual concentrations. Analysis of historic trends in ambient benzo(a)pyrene. Ambient concentration projections. Analysis of historic trends in emissions of benzo(a)pyrene. Emission projections. Deposition of benzo(a)pyrene. Reduction potential of MS for benzo(a)pyrene. Umweltbundesamt Vienna, 23 February

30 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials The annual mean target value and upper/lower assessment thresholds for B(a)P are: Target value: 1 ng/m³. Upper assessment threshold: 0.6 ng/m³. Lower assessment threshold: 0.4 ng/m³. Just over half of the MS have at least one monitoring station in exceedance of the B(a)P target value in Some MS have many monitoring stations in exceedance; Poland, Czech Republic and Austria have more than ten. The largest compliance gap was 23.6 ng/m³ at a new station (unknown station type) in Poland. Just over half of the MS have had a least one monitoring stations exceeding the target value between 2001 and There were insufficient data for trend analysis on the ambient trends between 2001 and 2010 (due to a lack of data for the earlier years). In the case of the United Kingdom risks to successful sampling were reduced by switching to daily sampling. The apparent step change in the UK data is important to note, as other Member States may have used USEPA TO4 based samplers previously and have changed to the compliant dust samplers operating within the PM 10 sampling convention. There is a decrease in B(a)P emissions between 2000 and 2009 in the majority of MS, with available data. However, there is a significant number of MS that show an increase in emissions during this period. There are not enough data on B(a)P deposition available to draw any conclusions on deposition. The problems and gaps encountered in the data are: No projections data (emissions and concentrations). Webdab emissions data are not available for all Member States. The lack of projections data is a significant gap as it means that there is no available information on likely future changes. There is more widespread exceedance of the target value for B(a)P than for the heavy metals. There are many exceedances in Poland and other Member States to the east of Europe. There are exceedances of the target value at some industrial stations and traffic stations but most of the exceedances are at background stations. The use of solid fuel for domestic heating is likely to be the main source associated with the exceedances. There are also more exceedances of the assessment thresholds than for the heavy metals. Many MS have not reported any B(a)P deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all Mercury Six groups of analysis have been carried out for Mercury: Analysis of current (2010) levels of Mercury annual concentrations. Analysis of historic trends in ambient Mercury. Ambient concentration projections. Analysis of historic trends in emissions of Mercury. 30 Umweltbundesamt Vienna, 23 February 2013

31 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Emission projections. Deposition of Mercury. According to DD4 the MS are required to report the concentration of mercury, but no target has been prescribed. MS will have developed their own assessment criteria, predominately for use for planning and industrial process permitting. There are few data available on measured mercury concentrations for 2010 and for the period 2001 to Many MS have not reported any data and nineteen of the forty eight stations reporting total gaseous mercury in 2010 are in the UK. Typical concentrations measured in MS with available data in 2010 were around 1 to 2 ng/m³, however the largest reported value in 2010 was 17.8 ng/m³ (at a UK station). This compares with the long term Environmental Assessment Level (EAL) published by the Environment Agency for England and Wales of an annual concentration of mercury of 250 ng/m³. There were insufficient data for trend analysis on the ambient trends between 2001 and 2010 (due to a general lack of data). Emissions of mercury decreased between 2000 and 2009 for the majority of MS. However, there is a significant number of MS that show an increase in emissions during this period. According to the CCE Status Report 2010 data, mercury concentrations are predicted to decrease between 2010 and 2020 for all MS (in the most ambitious scenario) (CCE 2010). However, for the least ambitious scenario emissions are predicted to increase for almost all of the MS and decrease for just one MS (UK). There are not enough data on mercury deposition available to draw any conclusions on deposition. The problems and gaps encountered in the data are: Airbase and Questionnaire 2004/461/EC data are both very incomplete. There are not many data available; not many MS have provided total gaseous mercury data in the 2010 Questionnaire 2004/461/EC. Further investigation may be needed into the reasons why so many MS have not provided total gaseous mercury data. Many MS have not reported any mercury deposition data. The reason for the lack of data should be investigated. The requirement and purpose of deposition measurements should be reviewed and either the number of stations could be increased or it might be decided that deposition measurements are not needed at all Reduction potentials There is only very limited information on reduction potential is available from official sources. The key issues for emissions reduction in decreasing order of priority are: a) Emissions of B(a)P from residential combustion. b) Emissions of B(a)P, arsenic, cadmium and nickel from industrial sources including power production. c) Emissions of B(a)P, arsenic and cadmium from road traffic. d) Emissions of B(a)P and arsenic due to a combination of sources in an agglomeration. Umweltbundesamt Vienna, 23 February

32 Service Request 6 final report Assessment of current AQ situations, projections, reduction potentials Data reported by MS in the Questionnaire 2004/461/EC and emissions data do not necessarily indicate that the same sources are important. In addition, national emissions can only provide an indication of possible sources. As the exceedances may be confined to small areas, on a local level further sources might be of relevance, which might not show a large contribution to emissions on a national scale. Task 4 provides more detail on sources (UMWELTBUNDESAMT 2012, section 5). The results from this section specifically feed into Task 4 (section 5). 32 Umweltbundesamt Vienna, 23 February 2013

33 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs 3 REVIEW OF ASSESSMENT METHODOLOGIES FOR РM 10, PM 2.5, HEAVY METALS AND PAHS 3.1 Key messages The initial part of Task 2 (section 3) was to review the collective experiences of the MS, this was a good opportunity for MS to share their information, which was met with varying success. As part of this task, some fundamental questions were asked about which PM metrics (fractions) are important. All presently applied metrics provide useful data to health policy. Generally, the Target and Limit Values have been derived from the evidence of epidemiological and toxicological studies and by discussion with expert groups at MS, EU and International level. The number of PM 2.5 monitoring sites does not yet fulfil the requirements of the AQD. Cooperation is very rare between MS to share rural background monitoring sites. According to present legislation, the PM assessment focuses on the measurement of PM 10 and PM 2.5 mass concentrations. This is based on the evidence for a strong linkage between the mass concentrations and health effects; however, health-effects could not unequivocally be attributed to certain PM fractions. Initial studies have shown that short time resolution measurements of Black Carbon (measured as BC or as EC), and UFP could be the key metrics for acute effects. The heavy metals and PAH are important with regard to longer-term exposure, but further work on metalloids and chromium speciation may be needed. To broaden information on traceable PM properties or constituents of PM and their health effects, extended measurement requirements in the MS are necessary. For the selection of new, additional measurands balance has to be found between the assumed health impact, and the existence of preferably traceable but at least well defined methods of monitoring method. BC is discussed as a pollutant with clear relation to health effects. Better understanding and definition of BC is needed, including the development of a reference method. The reference methods for PM 10 and PM 2,5 are not based on well defined measurands but on convention, and even thoroughly standardized still comprise considerable variability in results. Unfortunately this is also the case for all continuous methods currently available; consequently, a change of the reference method to a continuous one only shifts the problem without improving the situation. Based on present legislation, benzo(a)pyrene is assessed as a marker for all PAH and their carcinogenic potential. Further research is recommended to identify both the carcinogenic potential as well as the atmospheric levels of the PAH in the IARC list of carcinogenic substances. 3.2 Context Measurement of PM and speciated PM in the atmosphere is an extremely challenging task. There are a number of different measurement techniques available. Measurement harmonisation is dictated by Directives and Standards within a defined level of uncertainty. When comparing measurements of PM, this uncertainty needs to be considered, but it does provide a basis for comparison of the measurement made using different sampling and analytical technologies. Umweltbundesamt Vienna, 23 February

34 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs The pollutants covered by the present review have seen various developments since entry into force of the Directives: For PM10 and PM2.5, ambient air measurement techniques must currently comply with EN 12341:1998 and EN 14907:2005 respectively, or demonstrate equivalence to these methods by reference to the equivalence guide6 (European Commission 2010). Various continuous monitoring techniques have been introduced, but their equivalence with the reference method has only been recently demonstrated and only in a few locations across Europe. This demonstration of equivalence is also being undertaken during a period where our understanding of the limitations and variability of the reference method are becoming clearer. This is already a key discussion point and will continue to be so in the coming years. In addition, there is a growing archive of data for concentrations of many different particle size fractions and research into associated health effects. Couple this to the introduction of measurement techniques allowing the simultaneous measurement of several particle size fractions, the question arises as to which fraction(s) the focus for regulation should be laid on in the future. For heavy metals, ambient air assessment techniques used must comply with EN 14902:2005 ambient air quality - method for the measurement of Pb, Cd, As and Ni in the PM10 fraction. In addition monitoring instruments of these particulate metals must adopt a sampling system that has been assessed by and is operated in accordance with EN 12341:1998. Measurement uncertainty can be managed by appropriate calibration frequencies, extraction of reference standards and maintaining stability of sample flow throughout the sampling periods. Mercury techniques must comply with EN 15852:2010 which describes an automatic measurement method, however the standard allows for a manual equivalent. For polycyclic aromatic hydrocarbons (PAHs) in ambient air, monitoring techniques must demonstrate their equivalence to EN12341:1998. The sampling techniques employed are non-automatic sampling techniques which are generally high-volume systems. Since the introduction of the reference method EN15549:2008 it is likely that there may have been additional validation of sampling techniques with ozone denuders. As with particulate metal measurement, uncertainty can be managed by appropriate calibration frequencies, extraction of reference standards and maintaining stability of sample flow throughout the sampling periods. For polycyclic aromatic hydrocarbons (PAHs) in ambient air deposition, monitoring techniques must demonstrate their equivalence to EN15980:2011. The validation trial demonstrated that the funnel-bottle bulk collector provided the most reliable and robust results hence this was chosen as the standard collector. Cylindrical gauges and wet only collectors can be used to measure deposition of PAH provided equivalence can be demonstrated. In addition, for all PAH measurements, the question arises whether benzo(a)pyrene is the most appropriate marker or another PAH is a more suitable replacement. Also, is more research/discussion required to identify whether PM2.5 is a more suitable particulate size fraction to measure for PAH Umweltbundesamt Vienna, 23 February 2013

35 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs 3.3 Scope and general approach This task covers a wide range of technical questions as well as questions related to the selection of particle size fraction (for PM) and marker pollutant (for PAH). These questions are addressed by the following general approach: Collection and review of available literature, such as papers in peer-reviewed journals, other technical papers and reports by network operators. Discussion of specific questions with members of expert groups such as AQUILA 7 and CEN 8. Contacting network operators in Member States with specific questions on their practical experience with monitoring techniques, data quality objectives, siting of stations, equivalence testing, and other topics. External review of the draft report by selected experts (AQUILA, CEN etc.) In detail this task covers the following questions: Review information provided (section 3.4) regarding inconsistencies due to monitoring issues, fulfilment of the datasets of requirements of the AQD, additional monitoring not reported Evaluate fulfilment of data quality objectives (section 3.5) Comparison of reported monitoring stations to macroscale siting criteria (section 3.6) Evaluate strength and weakness of the reference methods (section 3.7) PM 10 vs PM 2.5 : health effects and monitoring aspect (section 3.8) Reference method vs. near-real-time information via non standardized continuous monitors (section 3.9) Availability of data for different particle size fractions and constituents (section 3.10) Suitability of benzo(a)pyrene as marker for PAH concentrations (section 3.11) Correlation between the pollutants of the AQD and DD4 (section 3.12) A questionnaire was sent to Member States in February 2012 to get further information on these topics. 3.4 Review information provided Does the data provided show inconsistencies which may be related to technical monitoring issues? The meta data for monitoring techniques used to provide measurements has been provided by MS alongside measurement data. This information has been extracted from AirBase, compiled in one data set and assessed in order to discover the distribution of various methods across all MS. It is important that detailed information about monitoring techniques are provided if we are to assess information relating to use of the reference method, equivalent methods and nonequivalent methods used to measure the relevant species across all member states Umweltbundesamt Vienna, 23 February

36 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs Using the limited information and resources available, an assessment was carried out to try to further differentiate methods into further graded categories and an additional category where the specific method was not provided. Five categories were defined by an air quality expert, Brian Stacey, based on his understanding of the methods (Table 3). The actual methods used could be divided into four categories, the reference method, methods that have demonstrated equivalence criteria to demonstration of equivalence criteria, methods that have not but are deemed good methods that have been shown to fail by a relatively small margin i.e., just outside the 25% uncertainty detailed in the guidance (e.g. 27%) and poor methods that have been defined not to be used even for indicative measurements. Later, the information was amended using information taken from equivalence testing campaigns across Europe in Belgium ( ), Germany ( ), Finland ( ), The Netherlands ( ) and the UK ( ) Table 3: Categories for evaluating equivalence of different PM monitoring methods. Equivalence Categories ID Description Example for PM 10 1 Reference method Leckel sampler 2 Demonstrated to be equivalent MetOne BAM 3 Good, but not equivalent TEOM 4 Poor Turnkey Osiris 5 Unknown Not possible to determine method* *This is either because the method has not been tested for equivalence or not enough information provided, i.e. beta attenuation which could relate to several different instruments Using data with >= 90 % data capture uploaded to AirBase, it is possible to show that 7.5 % of PM 10 data sets in 2009 was measured using the reference method and 24.4 % using an equivalent method % of the data sets were measured using a method that was outside the criteria set out in the GDE for 2005 and 2010, and no member states were found to be measuring PM 10 or PM 2.5 using a poor method (category 4) % of meta data is not sufficient to determine a method % of PM 2.5 data sets in 2009 with a data capture of 90 % were obtained using the reference method % and 25.3 % of PM 2.5 data sets were measured using equivalent and nonequivalent methods respectively. There were 43% of measurements that could be not be categorised as a result of data omission or limited information. 9 VMM (2011), Comparative PM10 and PM2.5 Measurements in Flanders, 2010 campaign. 10 TÜV Rheinland (2009), Report on suitability testing of the ambient air quality measurement system SWAM 5a dual channel monitor with PM10 and PM2.5 pre-separators of the company FAI instruments s.f.l for the components suspended particulate matter PM10 and PM Finnish Meteorological Institute (2010), Demonstration of the equivalence of PM2.5 and PM10 measurement methods in Helsinki 12 GGD Amsterdam (2008), Field Experiment on 11 Automated monitors 13 Defra and the Devolved Administrations (2010) UK Particulate matter equivalence trials data re-processed in accordance with the January 2010 version of the guide to demonstration of equivalence (GDE) 36 Umweltbundesamt Vienna, 23 February 2013

37 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs Do the datasets provided fulfil the basic requirements of the directives (data capture, QA/QC, etc)? The data submitted to AirBase almost completely fulfils the data quality objectives. It is possible to determine the data capture in two different ways. In the first year of a measurement it is often unlikely to have a full year of time coverage. It is clear that data capture provided to AirBase should be obtained from data sets with at least 90% data capture. The question is, what the data capture should be relevant to, for example for a first year sample starting on 1st June until December (i.e. time coverage of 50%): 1) The actual time coverage obtained i.e. 100% of 6 months 2) The annual year in full i.e. 50% of the calendar year Currently this decision is down to the interpretation of the MS and as such there is an inconsistent approach for calculating the data capture when you assess the time coverage from the start and end dates provided with the data. Using the questionnaire it has been possible to determine, in part, if member states are covered by ISO17025 accreditation for all measurements and across all networks if applicable. Only Cyprus, Greece, Ireland, Italy and Latvia are not covered by ISO17025 accreditation for any air quality measurements as detailed in the questionnaire. The Czech Republic, Estonia, The UK, Hungary, Luxembourg, Latvia, The Netherlands, Romania, Sweden and Slovenia are covered by ISO17025 accreditation for all measurements relevant to the Task 2 assessment (HM, B[a]P, PM 10 and PM 2.5 ). For the remaining countries, accreditation is either dependent upon the region or is unknown because no information has been provided Is there any other monitoring undertaken by the member states (additional sites or additional pollutants) that is not submitted to DEM? This section has been covered in section 3.10, please refer to this section for information relating to additional measurements. 3.5 Evaluate data quality objectives Analysis of reports available from network operators, including reports on equivalence testing Uncertainty The uncertainty of sampling methods for PM 10 and PM 2.5 can be determined by initial field measurements or during equivalence trials. To achieve a representative assessment to show the spread of sites across MS that are below 25 % uncertainty and those that are not for PM 10 and PM 2.5 we would need to be able to determine the method used to obtain the data uploaded to airbase. As the assessment of methods across all MS shows (see section 3.4), it is not possible to carry out an assessment in this way as there are currently too many methods categorised as unknown method as a result of omissions or the lack of more specific information. Umweltbundesamt Vienna, 23 February

38 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs Time Coverage There is no time coverage requirement in the AQD for PM 10 and PM 2.5 measurements; however it is necessary to ensure that the data capture (%) for all measurements is consistent to ensure that the data quality objectives are met. Recommendations have been made in light of a possible inconsistency that occurs with the provision of data capture in per cent as opposed to days Data Capture For 2009, 69 % of 2,851 PM 10 data sets achieved a data capture of 90 % or more. This is a 10% increase compared to The highest percentage (71 %) of data sets with data capture 90 % appeared in Only 53% of 801 PM 2.5 datasets achieved data capture 90 % in 2009, this is 10 % higher than in UK, Romania, Greece, Ireland, Latvia and Malta provided less than 50 % of PM 10 datasets with a data capture of 90 % for In Austria, Bulgaria, Finland, Lithuania, Estonia and Luxembourg 90% or more of the PM 10 data sets had 90 % data capture. UK, Spain, Poland, Romania, The Netherlands, Bulgaria, Croatia, Latvia and Malta show less than 50 % of PM 2.5 data sets with 90 % data capture. In Hungary, Austria, Slovakia, Slovenia and Cyprus all of the PM 2.5 data sets provided had 90% data capture Recommendations for improvements The findings surrounding missing documentation of sampling and analytical methods are a major issue when determining the station compliance with the data quality objectives. The Commission needs to police its own requirements for data provision thoroughly. Data sets without documentation of measurement methods cannot be used for assessment. MS should provide uncertainty information with the data; this could be checked with assumptions made using the first recommendation. Specific details of sampler manufacturer, model and analysis method (if applicable) should be provided for all measurements such that the equivalence can be categorised. It would also then be possible to list the uncertainties from equivalence reports and similar information such that assumptions could be made regarding the uncertainty of data sets. This could then be used as a sense check with the quoted uncertainty provided. Time coverage and data capture should be detailed in terms of days sampled as opposed to per cent so there is less possibility for error. I.e. Time coverage 365 days, Data capture 286 days. This has the following advantages: Verify the start date and end date corresponds with the time coverage Removes any potential inconsistency with the data capture 14 The comparably low fraction of PM 2.5 stations with high data capture can be attributed to the large number of new PM 2.5 stations put into operation during the year. 38 Umweltbundesamt Vienna, 23 February 2013

39 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs 3.6 Siting criteria This task comprises a comparison of reported monitoring stations to macro-scale siting criteria of the AQD as laid down in Annex III, V, VIII, and IX of the AQD for each pollutant: Annex III: Macro-scale and micro-scale siting criteria for all pollutants covered by the AQD except ozone Annex V: Number of monitoring stations per zone (all pollutants covered by the AQD except ozone), including ratio between traffic and background sites, and ratio between PM 10 and PM 2.5 sites. Annex VIII: Macro-scale and micro-scale siting criteria for ozone Annex IX: Number of monitoring stations per zone for ozone. In addition, the number of monitoring sites fulfilling the monitoring requirements laid down in Art. 6 (5) and Annex IV of the AQD (background measurements of PM 2.5 compounds) and Art. 5 (9) of DD4 (background measurements of heavy metals and PAHs in PM 10 and their deposition) as well as cooperation with other MSs have been screened. Data sources are both AirBase and the annual Questionnaires according to 2004/461/EC, as well as replies from a questionnaire distributed to MSs. The percentage of background monitoring sites for NO 2 and PM 10 varies considerably between different zones, from around 30 % up to 100 %. The percentage of background PM 2.5 sites is generally higher, corresponding to the focus of the AQD on population exposure. This reflects the quite different structure of monitoring networks even within one MS. The number of PM 2.5 monitoring sites does not yet fulfil the requirements of Annex V. It may be considered that the installation of monitoring sites is not yet completed, and AEI sites, which per definition are urban background sites, have been installed at first. In case of heavy metals, which are monitored at few industrial sites, the percentage of hot spot locations varies from 0 to 100 % per zone. This may be justified because background heavy metal concentrations are below the lower assessment threshold in most parts of Europe. Most MSs state in their replies to the questionnaire the complete fulfilment of the siting criteria laid down in Annex III. The justification for non-compliance with the micro-scale siting criteria mostly comprises technical reasons due to local circumstances, mainly concerning trafficrelated measurement at larger distance from kerb than 10 m. The minimum requirements for the number of NO 2 monitoring sites laid down in Annex V.A are fulfilled in almost all zones. The minimum requirements for the sum of the number of PM 10 and PM 2.5 sites are not fulfilled in most MSs. In all cases of non-compliance with the ratio of PM 10 /PM 2.5 monitoring sites (between 0.5 and 2.0 according to Annex V), this ratio is above 2, i.e. there is a broad lack of PM 2.5 sites. The high amount of missing PM 2.5 monitoring stations may be attributed to a delay in the implementation of AQD. The requirement for the ratio of traffic and background sites (between 0.5 and 2.0 according to Annex V) is fulfilled in all zones in only four small MS; it is not fulfilled in all zones in 14 of the investigated MS, in three MSs only 25 % of the zones comply with these requirement. In most cases of non-compliance, this ratio is below 0.5, i.e. traffic sites are missing. Annex V.C of the AQD lays down the minimum number of monitoring sites to assess compliance with the critical levels for the protection of vegetation in non-agglomeration zones: one site per 20,000 km² if the upper assessment threshold is exceeded, one site per km² if the Umweltbundesamt Vienna, 23 February

40 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs concentration is between the lower and the upper assessment threshold; no measurement is required if the concentration is below the lower assessment threshold. The information derived from the 2004/461/EC questionnaires related to monitoring sites to assess compliance with the critical levels for the protection of vegetation is inconsistent or incomplete in several MSs. Therefore a check of the fulfilment of Annex V.C based on a representative subset of MSs is not possible. The criteria of Annex V.C are fulfilled in eight MSs. Several MSs do not designate ozone monitoring sites to assess compliance with the critical levels for the protection of vegetation or designate only a small subset of non-agglomeration zones. The criteria for the number of ozone monitoring sites per zone laid down in Annex IX are fulfilled in all zones in nine MSs (out of the screened 19 MSs); eight MS fulfil the criteria in at least 50 % of the zones, and two in fewer zones. All 16 MSs, which replied to the questionnaire, monitor PM 2.5 compounds as well as HM and PAHs in PM 10 at a sufficient number of rural background sites. PAH background deposition measurements are performed in only 12 MSs, HM deposition measurements in 14 MS measurements. Cooperation with other MSs is very rare, it only concerns BE/NL and FI/SE. 3.7 Reference methods This section discusses the strengths and weakness of the various reference methods standardised by the European Committee for Standardization (CEN) for the measurement of concentrations of PM, heavy metals and PAH s in ambient air and deposition rates. Information sources are the documents and draft standards of CEN, reports and presentations of Member States experience given at AQUILA meetings as well as reports and comparison reports by the European Commission s Joint Research Centre (JRC) Reference methods for PM Currently, the reference methods for PM 10 (EN 12341:1998) and PM 2.5 (EN 14907:2005) are manual gravimetric methods and allow more than one volume flow rate. As the mass of the PM material is determinded by weighing the filter at specified conditions before and after sampling, an daily information update to the public is not possible. At present the methodology for monitoring PM 10 and PM 2.5 in ambient air is being harmonised in a single European Standard (pren 12341:2012) which merges the earlier EN 12341:1998 and EN 14907:2005. The main differences to the existing standards for PM 10 or PM 2,5 are: sampling with a flow rate of 2.3 m³/h (low volume sampler) only; method allows the use of sequential sampler equipped with automated filter changers; stricter conditions required in the weighing room: 45 % - 50 % relative humidity; required filter identification. The major sources of uncertainty of gravimetric PM measurement are effects of humidity on filters, the sampling flow rate and the lack of criteria for the performance of filter materials used. The stricter requirements for the weighing procedures of filters in pren 12341:2012 are the result of filter tests to address the effects of exposure of filters to high or varying relative humidities. 40 Umweltbundesamt Vienna, 23 February 2013

41 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs In most of the MS low volume samplers operating at a nominal flow rate of 2.3 m³/h are used, also common is a flow rate of 1 m³/h which is neither reference according to EN 12341:1998 nor EN 14907:2005 and 30 m³/h which is reference according EN 14907:2005 but not according EN 12341:1998. All MS except one use samplers equipped with an automated filter changer, suitable for stand-alone operation. The most common used filter types are filters made of quartz fibre followed by filters made of glass fibre. The requirements of pren 12341:2012 for monitoring of temperature and relative humdity in the weighing room and the balance resolution are at present not fulfilled in all MS Reference methods for total gaseous mercury and heavy metals and PAH in PM 10 The reference method for the measurement of total gaseous mercury (TGM) concentrations in ambient air is an automated method based on atomic absorption spectrometry or atomic fluorescence spectrometry (EN 15852:2010). The results of the validation programme by CEN showed that the uncertainty in the calibration of the instruments is a key factor. Therefore the CEN working group proposed the development of more accurate and repeatable calibration techniques for automatic instruments in future. The uncertainty of the mercury vapour pressure was not included because there is no scientific consensus on which is the best one to use. The measurement of heavy metals (reference method EN 14902:2005) and PAH (reference method EN 15549:2008) in PM 10 consists of two parts. First the sampling in the field by collecting the PM 10 fraction according to EN and second the analysis in the laboratory. Validation programmes by CEN included laboratory and field tests. The JRC intercomparison exercises focused on the analysis of the filters and showed good results for the reference methods of analysis for both, heavy metals and PAH. Degradation of benzo(a)pyrene during sampling in the presence of reactive gases like ozone or nitrogen dioxide is still under discussion. Up to the moment no ozone denuders applicable with the reference methods of PM 10 are commercially available. Consequently CEN recommends further measurements with and without ozone denuders of benzo(a)pyrene in ambient air to inquire the effect of degradation with respect to the complience of the limit value Deposition of heavy metals and PAH The reference methods for the sampling and analysis of the deposition of arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons are standardised by CEN in three standard methods, EN 15841:2009 (arsenic, cadmium, nickel), EN 15853:2010 (mercury) and EN 15980:2011 (PAH). As set out in DD4, Annex V, the reference method for the sampling of the deposition shall be based on the exposition of cylindrical deposit gauges with standardised dimensions. All three reference methods describe sampling with three different collectors (wetonly, bulk and Bergerhoff type of gauge) and two different analytical methods. Laboratory and field tests carried out by different CEN working groups showed the following results: Sampling with different collector types and sample preparation are the main factors in the uncertainty budget of deposition measurements. A different sampling strategy is needed for rural and industrial sites. The various analysis methods did not influence the results noticeable. Deposition is highly influenced by coincidental effects. Umweltbundesamt Vienna, 23 February

42 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs 3.8 PM 10 vs. PM 2.5 Four questions were considered in this task Which PM fraction is the most relevant from the point of view of documented health effects? Epidemiology is limited by the data and statistical tools available. As time passes more information and experimental evidence are provided and a greater understanding of the biological and physiological processes within the human body is now available. Acute morbidity and mortality may correlate with PM fractions and other pollutants (SO 2, NO x etc ); however, if all these components also correlate with each other it is difficult to ascertain which are more important. It is known that there is a correlation between PM 10 and health effects. PM 10 has PM 2.5 as a sub-fraction, which mainly contains primary aerosol species such as elemental carbon (EC) and organic carbon (OC), and secondary aerosol species such as sulphate, nitrate, ammonia, and some secondary OC. It is therefore necessary to understand as completely as possible the potential for health impacts associated with each size fraction or component in order to best judge possible abatement measures. Presently, both PM 10 and PM 2.5 sampling conventions are still important in relation to health effects. Black carbon (BC) is also important in relation to health effects. Ultrafine particulate (UFP) particle size and number count concentration may be important in relation to health effects. However, speciation of metals within PM 10 and measurement of anions, cations and EC in PM 2.5 will continue to be important as the knowledge base expands. The UNECE/WHO Task Force on Health Aspects of Air Pollution are still firmly committed to the need for a reduction in exposure to PM 2.5, due to the presence of combustion derived components to reduce population exposure and reduce the health effects seen (WHO 2012). The Task Force recommended that PM 2.5 remains the primary measure, with BC as a suitable additional indicator, specifically for localised measures to reduce exposure to combustion PM but accepts that work still needs to be done on standardisation of BC and EC measurements and that there is still need of further toxicological studies on PM and BC Is it feasible for monitoring network operators to monitor both fractions, taking into account the availability of new monitoring techniques? The network operator has to gather measurements to cover a number of measurement metrics required for PM 10 and PM 2.5 under the AQD; consistency in the approach is needed if the reference methods and the metrics in the AQD do not alter. However, if some of the measurement metrics are no longer relevant for the assessment of the risk to health, then some consolidation of instrumentation will occur. Dual channel and multiple PM analysers are already in use in research and in some MS monitoring networks. This would, over time, make it possible to rationalise the physical instruments that have multiple PM fraction and PM collection capability. Development of systems is driven by legislative requirements. 42 Umweltbundesamt Vienna, 23 February 2013

43 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs Is particle number a better metric than particle mass with respect to human health? On balance, measuring the particle number concentration for the UFP size ranges is important complementary to measuring the mass concentration of PM 2.5 and/or BC. Further studies may help better define the data requirements for health assessment Is there a need for new reference methods? The continued need for the combined PM 10 and PM 2.5 reference method is clear. Development needs to continue on the current methods for BC and EC. The EC standard is at the Technical Report Stage, there are a number of operationally determined definitions of EC, so there is still a lack of standardisation. For BC, there is a predominant but evolving method, but not true standardisation, with the existence of built-in sampling or artefact bias correction and post measurement correction regimes in publication, this can reduce the ability to compare data from researchers and current networks in operation in Europe and globally Conclusions The current weight of medical evidence strengthen the link between PM and adverse health effects. Epidemiologists have been presented with different metrics to which mortality and morbidity records can be compared, BS and SO 2 in the early 20 th Century, NO x, O 3 metals, PAH and PM 10 in the later 20 th Century and more recently PM 2.5, BC and UFP particle number and counting. Each has seen varying evidence of chronic and acute effects. At times a general indicator has been sought, such as BS, PM 10 and PM 2.5. The challenge has always been to elucidate what in the PM is having this effect. Researchers have hunted for a single factor, but in truth, there are many components of the PM that have the potential to present a risk to human health due to toxicity or other effect. Significant effort has been put into the operational definitions and sampling protocols for the constituent parts of the PM. Recent research has centred on understanding the effects of UFP, to understand the mechanisms in play, this would add to the number of determinations needed. Combined toxicological/epidemiological research is now picking apart this complex mix and may provide a means to rationalise the number of required measurements. Considerable attention is now being placed on Black Carbon, be it expressed as an optical property BC or as a thermal-optical property (EC/OC analysis). BC is being actively promoted by UNEP and WHO as a component to understand, measure and mitigate, to not only reduce localised health issues, but also to reduce the risk of climate change as BC is a recognised short-lived climate forcer. However, current scientific knowledge is not sufficient to implement standards for constituents such as BC and UFP. Presently, CEN is preparing a revision of the now combined PM 10 and PM 2.5 reference method that will continue to be important especially for the subsequent speciation of the PM. CEN is also preparing a standard for EC/OC to provide a platform for comparable data. The preparation of a standard for BC does need to be considered. However it has to be kept in mind that all these constituents are defined by convention of the measurement method. WHO is preparing to report on further studies of BC as a health indicator, which coupled with the climate change mitigation for control based on BC measurement and reduction could be a potential game changer in the near future. The decrease in mortality expected in Europe due to Umweltbundesamt Vienna, 23 February

44 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs controls based on BC attenuation is reasonable, but on a global scale outside the EU in the developing world, this would have far reaching implications. This does suggest that, in the medium term, PM 2.5 would be a reasonable sampling convention to retain for comparison with the derived limit values, and this is the current recommendation from the WHO. The understanding and measurement of BC and EC/OC needs to be expanded as does the toxicology of UFP; so that the standards and target values can be derived to augment or even replace the PM mass concentrations as the current measure in the future. 3.9 Reference method vs. near-real-time information The reference methods given in the AQD for the measurement of particulate matter (PM) are not commonly used for operation in routine monitoring networks. In order to fulfil the requirements of the Directive (information should be updated on an hourly basis), these networks usually apply Automated continuous Measurement Systems (AMS). The AQD allows the use of such systems after demonstration of equivalence with the reference method, i.e., after demonstration that these systems meet the data quality objectives for continuous measurements. Guidance on the demonstration of equivalence was provided by the European Commission (EC) Working Group on Guidance for the Demonstration of Equivalence (most recent report from 2010, EUROPEAN COMMISSION 2010).This means that there are requirements and guidance for the use of AMS, but there is no standard method for continuous PM monitoring. Given the fact that the allowed uncertainty for PM measurements is as high as 25%, that the reference method itself is associated with uncertainties (see section 3.7), and that Member States use different kinds of AMS in different configurations, it is evident that variation in PM measurements is relatively high, both within and between Member States Are there any implications associated with the fact that there is no standard method for continuous PM monitoring? A consequence of not having a standard method is that there is a lot of variation in the type and configuration of AMS used in monitoring networks. There are differences between Member States, but also within some Member States. Based on the information provided by Member States to the dedicated questionnaire, some Member States apply many different types of AMS within their monitoring networks (for example Austria and Spain). In the UK one type of AMS is applied, but with different sampler dryer configurations (RICARDO AEA 2011). AMS may be based on the use of oscillating microbalances (TEOM) or ß-ray attenuation, and on in-situ optical methods (e.g. Grimm dust monitor). Most Member States apply TEOM or ß-ray monitors. The performance of AMS (and the deviation from the reference method) depends on many variables: Configuration of the system e.g. inlet heating, filter material, either or not fitted in a conditioned housing Composition of the aerosol depending on the type of monitoring station (traffic, urban, industrial, rural) share of volatile components Meteorological conditions temperature, relative humidity 44 Umweltbundesamt Vienna, 23 February 2013

45 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs wind speed (performance of the sampling head) e.g. research in the UK (HARRISON et al. 2010) showed that the TEOM FDMS overestimated the PM concentration especially on days with temperatures higher than 25 C, but not on all of those days. There may be a relation with relative humidity (inefficient drying). Maintenance condition and age of the system e.g. preliminary evidence collected to date suggests that the TEOM FDMS analyser baseline responses can change by 4 μg/m³ when a new dryer is installed (RICARDO AEA 2011) The equivalence trials that are required to determine the instrument uncertainty, do not give insight in long term operational roll out of a candidate method. This has been acknowledged by the CEN TC 264 Working Group 15 that is in the process of developing a standard (or technical specification), see under Question 4, section Data acquisition method e.g. comparison of a large number of monitoring stations in the Netherlands (with ß-ray attenuation systems) showed that data acquired digitally were more in line with data from the reference method than analogue data. Deviations in the analogue data ranged from -2 to +4 μg/m³ (RIVM 2007). Apart from these, there may be other variables that we currently are not aware of. The implication is that inevitably there is a lot of variation between raw measurement data from AMS. The variation can be decreased by applying procedures for equivalence demonstration. However, these procedures may vary substantially between Member States, e.g. in the number and variation of monitoring locations that are taken into account, how often a procedure is repeated, the number of instruments, etc. Also, Member States report that the availability of reliable AMS is limited. In the questionnaire, the UK mentions: There are severe limitations in terms of the availability of automatic techniques which are reliable, type approved, proven equivalent, are tried and tested in the field and for which the monitoring method is transparent and well understood. Experience has shown that, over the long term (that is, outside the scope of equivalence trials) there are issues around the intercomparability of different measurement methods and thus a mixed network, and that all PM monitoring techniques have their own quirks and problems Is there any information to suggest that the relationships between continuous and gravimetric samplers remains constant with time? Given the list of variables that the performance of AMS depends upon under question 1, and the fact that those variables may vary over time, the answer to this question clearly is that the relationships are not constant with time. In more detail, the following plays a role in the variation in the relationship with time: Due to new insights, the configuration of AMS applied in monitoring networks changes with time (e.g. RIVM 2007). Due to new insights, the choices that are allowed by the EN for the reference method may change with time (e.g. filter type material, conditioning of housing). Replacement of analyzer s components following maintenance schemes may result in a change of the signal (e.g. with respect to dryers). For an FDMS analyzer, changing even apparently minor components (like rubber air seals) can materially affect performance (RICARDO AEA 2011). Umweltbundesamt Vienna, 23 February

46 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs When an analyzer needs to be replaced at the end of its lifetime, a direct like for like replacement will often not be possible (due to changes in the configuration by the manufacturer). The share of volatile components varies over time. Meteorological circumstances (temperature, humidity) vary over time. Besides the temporal variation, the relationship between continuous and gravimetric samplers also vary in space. The order of variation seems to depend on the type of monitoring station and the type of analyzer. In an intercomparison study in Germany it was shown that for both PM 10 and PM 2.5 measured with TEOM FDMS, the relationship may vary drastically from site to site. However, there was almost no variation in the results obtained with the SHARP monitor (PFEFFER et al. 2011). An intercomparison study in the Netherlands also showed that the relationships vary more for certain types of analyzers (RIVM 2008). A further report by RIVM established correction equations for PM 10 measured with ß-ray attenuation analyzers in the Dutch monitoring network (RIVM 2008a). They differ between the rural and urban stations. It seems therefore important that Member States derive correction equations for the different types of location. This requirement will likely be implemented in the new standard for AMS (for traffic, urban, industrial and rural stations), developed by CEN TC 264, WG 15 (see under question 4) Does this render information to the public more difficult? Daily mean PM 10 concentrations, and the resulting number of exceedance days have to be published every day. These data have not been validated following procedures of the monitoring authorities. In most cases, the validation will only take place after the year has ended. This may result in a substantial change in the number of exceedance days once the year has passed. It is hard to explain this to the public, especially when the number of exceedance days decreases What would be the advantages/disadvantages of a separate, continuous standard method? As mentioned under question 1 (section 3.9.1), procedures for equivalence demonstration may vary substantially between Member States. This has been acknowledged by the European Commission. Currently, the CEN TC 264 Working Group 15 is in the process of developing a standard (or technical specification), under the working title Ambient air quality Automated continuous systems for the measurement of the concentration of particulate matter (PM 10 ; PM 2.5 ). Currently, the standard aims at the following: Laying down the minimum performance requirements and test procedures for the selection of appropriate AMS for particulate matter (type approval). This includes the evaluation of equivalence with the reference method. Describing minimum requirements for ongoing quality assurance quality control (QA/QC) of AMS deployed in the field. Describing requirements and procedures for the treatment and validation of raw measurement data that are to be used for the assembly of daily or yearly average concentration values. Especially the second aim seems important, since relationships between continuous and gravimetric samplers do not remain constant with time (see question 2, section 3.9.2). 46 Umweltbundesamt Vienna, 23 February 2013

47 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs The disadvantage of a standard that only gives minimum requirements is that there will still be a lot of variation in measurement results for PM. To minimize the variation, a standard would be needed that also defines the measurement method and configuration of the AMS. However, the still ongoing research into the performance of both AMS and the reference method on the one side and the allowed uncertainty for PM measurements of 25% on the other, would not allow for a standard that excludes certain types of AMS Particle size fractions Data from the informal questionnaire circulated to Member States (section ) was used together with data that had been supplied or obtained from Member States on measurements other than PM 10 and PM 2.5. The level of detail provided by the Member States was not consistent and ranged from very succinct descriptions to incomplete forms. Some Member States included actual data along with their completed informal questionnaire. A summary of these replies is given in Table 4. Table 4: Summary of responses by MS to the informal questionnaire on PM other than PM 10/PM 2.5. Member State PM 1 UFP Particle Numbers OC EC Inorganic Carbon BC Anions Cations Austria y n n n y (nd) n n y (nd) y (nd) Belgium y y (2011) y (nd) y (nd) y (nd) n y y (nd) y (nd) Bulgaria Croatia unavailable unavailable Cyprus n n n n n n n n n Czech Republic n n n y y n n y y Denmark n n y n n n n n n Estonia n n n y (2011) y (2011) n n n n Finland unavailable France n y n y y n y y y Germany n n y (nd) n n n n n n Greece n n n n n n n n n Hungary unavailable Ireland n n n y (2011) y (2011) n n y (2011) y (2011) Italy y y (2012) y (2012) y (2012) y (2012) y (2012) y (2012) y (2012) y (2012) Latvia n n n n n n n y (nd) y (nd) Lithuania n n n n n n n n n Luxemburg n n n n n n n n n Malta unavailable Netherlands n n n n n n y n n Poland n n n y y n n y y Portugal unavailable Romania n n n n n n n n n Slovakia unavailable Slovenia n n n n n n n n n Spain y n n y y n n y y Sweden n n y (nd) y (nd) y (nd) n y (nd) n n United Kingdom n y y y y n y y y y = species measured and data available y (2011) or y (2012) = measurements only started in 2011 or 2012 y (nd) = species listed as measured, but data not given n = species not listed as measured Umweltbundesamt Vienna, 23 February

48 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs The following Member States did not reply to the informal questionnaire: Portugal (PT), Bulgaria (BG), Slovakia (SK), Finland (FI), Croatia (HR) and Malta (MT) The following Member States replied, but do not undertake any further PM size fraction or speciation measurements other than the gravimetric assessment of PM 10 and PM 2.5 required under the Directive. They currently do not possess any plans to change/amend this strategy in future years: Romania (RO), Slovenia (SI), Cyprus (CY) and Luxemburg (LU). The following measurements are being conducted by the remaining Member States: PM 1 This is a dust sampling convention analogous to PM 10 or PM 2.5 but with a sampling inlet with a 50 % efficiency cut off at 1 µm mean aerodynamic diameter. This is typically measured by a light scattering technique rather than by direct manual measurement. Ultrafine particle size (UFP) distribution and number count typically for the observation of particle numbers in size classes less than 1 µm in diameter (number concentration of particles) Elemental carbon (EC) and organic carbon (OC) are measured by thermal -optical analysis with transmittance or reflectance correction. EC/OC are required in the speciation of PM 2.5 in the Directive. Black carbon (BC) is measured typically using an Aethalometer in the infrared range (wavelength of 880 nm). Black smoke measurement was an atmospheric dust pollutant method that pre-dates the current BC measurements now in more common use. UV carbon UV carbon is not a true physical parameter but determined, using an Aethalometer at a wavelength of 370 nm less the BC concentration. In the ultraviolet region below 400 nm increased absorbance is shown for some organic carbon and fine smoke (diesel, oil fume, solid fuel emissions and tobacco fume). Anion and cation speciation are determined using time-integrated filter sampling and by continuous denuder/ion chromatography systems of varying complexity (multiple PM 2.5 systems to large dual PM 10 /PM 2.5 /gas analysis systems). The AQD requires the speciation of SO 4 2, NO 3, Cl anions and Na +, K +, NH 4 +, Ca 2+, Mg 2+ cations in PM 2.5. The following Member States provided information on PM monitoring other than PM 10 and PM 2.5 : Other PM fractions: Continual UFP measured at one location in Germany, France and Italy, two sites in Belgium and Sweden, three locations in Denmark and four locations in the United Kingdom. Where data was provided, this was included in the Task Chapter. BC is measured at four locations in France (FR) and Sweden (SE), 20 locations in Belgium (BE), 21 locations in the United Kingdom (GB); The Netherlands (NL) are currently measuring Black Smoke. PM 1 is measured at one sites in Austria (AT), two sites in Italy (IT), multiple sites in Wallonia in Belgium (BE), and 25 sites in Spain (ES), Other species within the PM fractions: EC/OC were measured at one site in Spain (ES), Poland (PL), Belgium (BE), the Czech Republic (CZ), Austria (AT) - EC only, Ireland (IE) and Estonia (EE); two locations in Italy (IT) and Sweden (SE); four sites in the United Kingdom (GB) and 15 urban measurement stations in France (FR). Anions and cations were measured at one site in Spain (ES), Poland (PL), Belgium (BE), the Czech Republic (CZ), Ireland (IE) and Latvia (LV), two sites in Italy (IT), four sites in the United Kingdom (GB) seven sites in Austria (AT) and at 15 urban measurement stations in France (FR). 48 Umweltbundesamt Vienna, 23 February 2013

49 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs 3.11 Benzo(a)pyrene as marker For the purposes of assessment under DD4, benzo(a)pyrene (B(a)P) was to be measured and compared against the prescribed limit value of 1 ng/m³ B(a)P is defined as a human carcinogen by the International Agency for Research on Cancer. In addition to B(a)P, at least six other specified PAH were also to be measured: Dibenz(a,h)anthracene (DbA) - defined as a probable human carcinogen and Benzo(a)anthracene (BaA), Benzo(b)fluoranthene (BbF), Benzo(j)fluoranthene (BjF), Benzo(k)fluoranthene (BkF), and Indeno(1,2,3-cd)pyrene (IdP) these are all defined as possible human carcinogens. Like B(a)P, the benzo fluoranthenes and dibenz(a,h)anthracene are all five ring PAH structures, benzo(a)anthracene has four rings and Indeno(1,2,3-cd)pyrene has six (Figure 4). B(a)P DbA BaA BbF BjF BkF IdP Figure 4: Chemical structure of PAH (source: Wikimedia Commons). Benzo(a)pyrene was selected as a marker both by the EU and by other bodies. It has a long history of characterisation and assessment. Data collected by the Member States could be used to verify the selection of B(a)P. The available annual mean data from all Member States was assessed for correlation between B(a)P and the other reported PAHs, more significant correlations were found than significant anti-correlations. However PAH has a strong seasonal variation, with the highest mass concentrations between early December and mid February, the summer months being at negligible levels. Data was taken from the United Kingdom from measurements using the DHA80 PM 10 sampler. Correlation between B(a)P and the six individual selected PAH is very good, out of 32 sites where the monthly data from at least 2008 to end of 2011 was made available, using typically, 46 pairs of data, 30 sites had very significant correlations, with the remaining two with significant correlations. The same calculations correlating BkF against each of the additional PAH gave a very similar outcome. It is by no means any validation of the use of B(a)P as a marker, as in the literature, the selection of B(a)P as the marker has come under scrutiny. Two key papers by Park and Saarnio provide good evidence on the probable list of minimum PAH that are useful to measure and also for Umweltbundesamt Vienna, 23 February

50 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs the use of benzo(k)fluoranthene as an alternative marker for the possible and probable carcinogenic PAH (PARK et al and SAARNIO et al. 2008). However, Saarnio focuses on other factors, such as the relative difference in stability of B(a)P, which is considered more reactive than BkF. For the UK dataset, we have substituted BkF for B(a)P in the correlation calculations and was not really any different to the results obtained from B(a)P against the required additional PAH.. So as far as a surrogate of the six PAH measured under the Directive, B(a)P and BKF would both suffice, but a risk based limit value has already been assigned to B(a)P. Each PAH will have a relative toxicity relative to B(a)P, there are many in the published literature, but with some widely differing ranges and further complications of derived carcinogens from the reactive lighter PAHs and PAH present in different particle fractions, a weighting system for a range of PAH would be difficult. From the AirBase data and the available high resolution data from the United Kingdom, there is nothing to suggest that B(a)P is not a suitable marker with regards to overall apparent behaviour. This suggests that a marker is still appropriate. The list of additional PAH does miss some commonly measured PAH, which are useful in ratio profiling for source apportionment, a larger profile is also useful for the alternative method of profile signatures. Although short term measurement campaigns may be better suited for localscale source apportionment, researchers have successfully used National Network datasets to achieve useful national level source apportionment (TOBISZEWSKI et al. 2012, MARI et al DVOSKA et al., 2012, GALARNEAU 2008 and SAARNIO et al. 2008). To facilitate the basic source apportionment ratios, this would suggest the inclusion of phenanthrene, anthracene, pyrene, fluoranthene and benzo (ghi) perylene. The ratios of these selected PAH species can be used to broadly characterise the possible influences from coal combustion, diesel exhaust fume, petrol exhaust fume, natural gas combustion, oil combustion, vegetative combustion and wood combustion. However, there are some overlaps between these various PAH ratios Relationships between pollutants Correlations between the pollutants PM 10, PM 2.5, As, Cd, Ni and B(a)P were calculated from the data in AirBase. The significant correlations and anti-correlations are summarised in Table 5. There were no significant correlations between the data for PM 2.5 with B(a)P, Cd or Ni, or B(a)P with Cd or Ni. Table 5 provides a summary of the correlations, this shows the number of sites that are colocated for each of the correlations, the number of sites having n years of paired data and the number of results that are potentially significant correlations and anti-correlations (i.e. where the correlation was at or above the 95% confidence interval) and also shows the number of sites were there was a positive or negative tendency. 50 Umweltbundesamt Vienna, 23 February 2013

51 Service Request 6 final report Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs Table 5: Summary of correlating and anti-correlating measurement data (number of sites). Assessment Correlating sites Anti-correlating sites PM 10 vs As AT: 1, DE: 1, DK: 1, IT: 1 AT: 1 PM 10 vs B(a)P AT: 5; LT: 1 IT: 1 PM 10 vs Cd AT: 1, DE: 2, DK: 1 PM 10 vs Ni AT: 1, DK: 2, IT: 1 DE: 1, IT: 1 PM 10 vs PM 2.5 AT: 4; BE: 1; CZ: 16; DE: 6; ES: 2; FR: 2; GB: 1; HU: 1; IT: 6; LT: 1; PT: 4; SE: 1 PM 2.5 vs As DE: 1 B(a)P vs As AT: 1 BE: 1 As vs Cd AT: 1; BE: 2; DE: 1; LT: 1; UK: 10 AT: 1; BE: 2; UK: 1 As vs Ni AT: 1; BE: 2; DE: 2; DK: 5; IT: 3; UK: 4 AT: 1 Ni vs Cd DK: 1; IT: 1; UK: 4 AT: 3; BE: 1 Where there was collocated data for multiple pollutants, these were also assessed together; it was found that there are four sites where three measurement parameters all correlate strongly. These were at two sites in the United Kingdom for As, Cd and Ni at GB0047R Heigham Holmes (rural background) and GB0792A Sheffield Brinsworth (urban); and one site each in Italy IT1523A D Acquisto (urban background), Asti for Ni, As and PM 10 and Denmark DK0051A Arhus (urban traffic) for Ni Cd and PM 10. It was hoped that the correlation of these pollutants would provide information on the sources and to discuss how these sources may be addressed. Additional information and measurements would be required to detail a complete source apportionment for each Member State. Possible correlations between PM 10, PM 2.5, As, Ni, Cd and B(a)P can be attributable to multiple sources and processes. Identification of individual sources would be a complex task requiring a much more detailed assessment of each monitoring site and the industry and roads local to them, including extensive source receptor modelling and finer resolution data. A more detailed analysis of sources is undertaken in the specific report for Task 4, see a summary in chapter 5.6 (UMWELTBUNDESAMT 2012). For PAHs other than B(a)P suggested in DD4, this list omits a number of PAH that can be used for source apportionment as considered in Section 3.11 above. Umweltbundesamt Vienna, 23 February

52 Service Request 6 final report Developing future objective(s) for PM2.5 4 DEVELOPING FUTURE OBJECTIVE(S) FOR PM Key messages The Air Quality Directive requires the review of the PM 2.5 standards, including investigation of the feasibility of a more ambitious limit value. Changes of PM standards could improve the effectiveness of health protection, but such improvements should be carefully balanced against the importance of regulatory stability. Possibilities of changing properties of current standards have been investigated, such as the binding nature of the National Exposure Reduction Target and the spatial extent of the Average Exposure Indicator and recommendations have been given Possibilities for new PM standards have been investigated, this is not recommended Possibilities for simplifying the set of PM standards have been investigated. Withdrawal of PM standards is however not in accordance with the WHO recommendations. First results of the current evaluation of PM by WHO and model projections of PM concentrations by IIASA results could be taken into account, but full analysis of attainable levels was not possible. 4.2 Context Article 32 of the AQD obliges the Commission to review the PM 2.5 air quality standards in the light of new information and to take into account the feasibility of adopting a more ambitious limit value for PM 2.5, to review the indicative limit value of the second stage for PM 2.5 and to consider confirming or altering that value. Task 3 of this project, which is summarized in this chapter, aims to support this review (TNO, UMWELTBUNDESAMT & RICARDO AEA 2013). New scientific information about the health impact of PM was obtained from the recommendations by WHO (WHO 2012a, 2013). Data on air quality levels in Member States were based on the review in Task 1 (section 2) and on model calculations by IIASA aimed at possible revisions of the NEC. Task 1 also gave information on the progress made in the reduction of PM 2.5 emissions and ambient concentrations resulting from Community measures, and this information was supplemented by the results of a recent questionnaire for the member of the Air Quality Committee on the implementation of the PM 2.5 provisions. In response to a previous questionnaire to the Stakeholder Expert Group on the Air Policy Review and in a recent workshop on PM, Member States and other stakeholders have suggested considering revision of the PM standards. These suggestions included simplification of the set of PM standards, options for including Black Carbon or Ultrafine Particles, and diverging possibilities of making the standards more or less stringent and more or less flexible. Based on this information and other relevant information, strengths and weaknesses of the existing and possible new PM air quality standards were evaluated and recommendations on possible revisions of the PM standards were developed. 52 Umweltbundesamt Vienna, 23 February 2013

53 Service Request 6 final report Developing future objective(s) for PM Identification possible new PM standards and selection for further investigation Criteria for air quality standards In order to judge the feasibility of air quality standards, a substantial number of relevant criteria needed to be taken into account: Health protection in particular the potential health benefits triggered by actions to achieve the standard, Cost-effectiveness of action driven by the standard, Attainability and attainment costs, Scientific robustness, Environmental equity, Fairness to regulators (e.g. differences in reduction potentials, in effort already undertaken, differences in climate and topography) Regulatory stability/continuity, Possibilities to assess (measure/model) compliance, Coherence with other (EU) legislation (e.g. EURO regulations for mobile sources), Synergy (or antagonism) regarding other (EU) policies, Stability in relation to meteorological variability, Comparability to international standards, Implementation burden, Redundancy, Complexity, Message conveyed and transparency. The criteria were used to evaluate the added value of possible changes given the existence of the current set of PM standards. Using the above criteria we discussed whether a change was favourable, neutral or unfavourable. We did not attempt balancing the added value against the regulatory stability criterion, which is always a reason for not changing the legislation. Changes that we identified as possible improvements of the PM standards were recommended for consideration, but the choice between improving the current provisions or leaving the system unchanged was left to the political decision making process. Acceptability for stakeholders, in particular Member States, is obviously another important criterion. However, because the current investigation is intended to support the stakeholders in finding an acceptable set of PM standards, this criterion was not considered explicitly Selection of possible new PM standards for further investigation Air quality standards comprise a number of properties that together define the standard: the PM fraction, the binding nature, the level to be attained, the attainment date, temporal aspects (averaging period) and spatial aspects. In the Air Quality Directive most of these properties are explicitly written as part of the definition of the standards, but some other properties are defined elsewhere in provisions that relate to the standard. In Task 3a (section 4.3) we selected for each of these properties options for further investigation in Task 3d (section 4.6). Umweltbundesamt Vienna, 23 February

54 Service Request 6 final report Developing future objective(s) for PM PM fraction The options for PM fractions will primarily be based on the recommendations by the WHO; a PM fraction will only be considered if there is sufficient evidence of its health risk. Stakeholders and international scientific organisations have recommended considering regulating BC/EC (see also section 3.8). In the USA a standard for coarse particulate matter PM has been introduced 15. Indicators selected for further evaluation: PM 2.5 PM 10 PM BC/EC Binding nature The binding nature of a standard is closely linked to the level to be attained and to the levels that are achievable under different scenarios for future emissions; the level to be attained can be set lower when the binding level is reduced. In view of uncertainties in the attainability of new standards, the binding nature may be very important for stakeholders. Therefore we will keep all possibilities for further evaluation. Binding options selected for further evaluation: Binding standards (limit values, the ECO), which set air quality levels that have to be attained by a given date, Derogations of binding standards, Target value, which does not require measures entailing disproportionate costs, Short-term alert and information thresholds Alert threshold, Stage 2 standard and timeline, Long term objective, Non-binding health indicator Level to be attained The level to be attained can be a specified concentration or a specified change of the concentration (an absolute change or a percentage change). Some stakeholders have suggested considering a standard for the national contribution to the concentration, excluding transboundary contribution, which cannot be controlled by the responsible authorities. The level that can be attained in 2015, 2020, 2025, 2030 and possibly 2050 will be based on calculations by IIASA. Parameters of levels to be attained selected for further evaluation: Concentration; Percentage change in concentration; National contribution to concentration; Percentage change to national contribution to concentration. Numerical values of levels to be attained: No restrictions Umweltbundesamt Vienna, 23 February 2013

55 Service Request 6 final report Developing future objective(s) for PM Attainment date Data on attainability will be available for 2015, 2020, 2025, 2030 and possibly There is no reason to exclude at the first stage any attainability date. Attainability dates selected for further evaluation: No restrictions Temporal aspects The choice of the temporal aspects will in the first place be based on the WHO recommendations. Temporal aspects preliminarily selected for further evaluation: Annual averages Multiyear averages; Percentiles of daily averages Spatial aspects The spatial extent of the current limit values is implicitly given by the siting requirements of monitoring stations. The spatial extent of the NERT and ECO is defined in the AEI. When a standard applies everywhere, the attainable level is high because it depends on the most unfavourable locations in the EU; for the many other areas where such a high limit value would be already met, the directive does not require action. Therefore more spatially differentiated limit values should be considered. Stakeholders have suggested relating standards more strongly to human exposure. Spatial aspects selected for further evaluation: Applying everywhere, as for the current limit values; Depending on the type of location, particularly urban background; Spatially averaged over certain types of area; Related to human exposure. 4.4 Evaluating the current state of implementation of the relevant provisions Implementation of assessment provisions The current state of implementation of the provisions relevant to PM 2.5 were evaluated in Task 1 of the current project. Data from Airbase, the annual questionnaire 2004/461/EC were considered along with emissions data. Responses to a questionnaire to Member States in February 2012 seeking further information were evaluated. Five groups of analysis have been carried out for PM 2.5 : Analysis of current (2010) ambient PM 2.5 annual mean concentrations Analysis of historic trends in ambient PM 2.5 concentrations Analysis of historic trends in emission of PM 2.5. Umweltbundesamt Vienna, 23 February

56 Service Request 6 final report Developing future objective(s) for PM2.5 The calculation and assessment of the Average Exposure Indicator (AEI). Analysis of PM below PM 2.5 and constituents. The results of this analysis are summarized in section 2.4 and Implementation of management provisions Since the introduction of the PM 10 limit value, numerous measures have been implemented in most Member States to achieve compliance with those limit values. These measures have inter alia reported in time extension notifications. As the USA has had air quality standards in place for PM 2.5 for some years, as a starting point, we considered the extensive list of actions published by the US EPA 16 as reasonably available control measures for PM 2.5. We then considered the EU management provisions for PM 10 standards and mapped these onto those known to deliver PM 2.5 emission reductions, based on the US EPA experiences. Hence, we have examined those measures being implemented to reduce PM 10 emissions according to: Type of exceedance area, i.e. whether it is predominantly vehicular, industrial, or domestic emissions that are responsible for potential non-attainment; Source sector and type of measure applicable; The timescale for implementation (short or long term) Whether a source/measure combination is likely to assist with meeting a PM 2.5 National Emission Reduction Targets (NERT), the Target Values (TV) or limit values (LV) at the roadside; (i.e. whether the measure targets a reduction in the urban background or at hot spots, either roadside or industrial); How the impact of the measure is being monitored. We have also distinguished between options for PM 10 control and consequently PM 2.5 levels according to whether they focus on reducing primary sources of PM or whether they reduce secondary PM as well. In addition we highlighted measures that mainly reduce PM 10 but are of limited effect in the case of PM 2.5 such as street sweeping or winter sanding restrictions. Where possible we have drawn on recently published examples from a limited number of European countries (selected from the TEN) to illustrate the range of approaches followed in the wider EU. There is little context specific information on the cost effectiveness of measures that which is available is highly unsystematic and is illustrative mainly of the problems of collecting sound financial information. The detailed description of measures can be found in the specific report for Task 3 (TNO, UMWELTBUNDESAMT & RICARDO AEA 2013) Measures suitable for exceedance situations where vehicular exhaust emissions dominate In general, exhaust emissions occur in the fine fraction; therefore measures to reduce exhaust emission reduce PM 10 and PM 2.5 emissions to the same amount Umweltbundesamt Vienna, 23 February 2013

57 Service Request 6 final report Developing future objective(s) for PM2.5 Actions shown to reduce PM 2.5 emissions from vehicles are given in Table 6. These actions were mapped onto measures commonly deployed in the Member States to reduce PM 10 emissions and encompass the following measures: Low Emission Zones Public Procurement Policies Traffic Management Encouragement of Modal shift Other transport measures e.g. provision of electric vehicle charging points. Table 6: Additional actions that have been demonstrated to reduce PM 2.5 emissions from vehicles according to the US EPA. Mobile Source Actions On-road diesel engine retrofits for public service and heavy goods vehicles using Euro standards Non-road diesel engine retrofit, rebuild/replace with catalysed particle filter Diesel idling programs for HGV, locomotive, and other mobile sources Transportation control measures including transportation demand management and transportation systems management strategies Programs to reduce emissions or accelerate retirement of high emitting vehicles, boats, lawn and garden equipment Emissions testing and repair/maintenance programs for on-road vehicles Emissions testing and repair/maintenance programs for non-road heavy duty vehicles and equipment Programs to expand use of cleaner burning fuels Opacity/emissions standards for ``gross-emitting'' diesel equipment or vessels NOTE: These actions are additional to those taken to meet extant legal obligations. All of these actions also reduce PM 10 and NO x emissions. Low emission zones Low Emissions Zones (LEZ) can be an effective way of reducing PM 10 and soot emissions that have the added value of reducing PM 2.5. LEZs are in place in 11 European Countries 17. They were first introduced in Sweden in 1996 and the first motorway LEZ was established in Austria in An increasing number of cities are implementing them, either for all vehicles or for heavy goods vehicles (HGVs) only. LEZs that are for HGVs will in general be less effective than the LEZs for all vehicles at least in inner city areas. Also those zones which were introduced early, covered a relatively large geographical area, set an ambitious emissions standards (Euro 4 and better), and which are strictly enforced are, of course, the most effective. A possible downside is that banning of high emitters in one location may relocate them elsewhere instead of reducing them and so might have an impact on hot spots without reducing overall background emissions; this would be a case where the action of a Member State would be unhelpful with meeting a PM 2.5 NERT. However, if the LEZ zone is large enough, vehicles will be affected on a much larger area as most of the vehicles might have to pass through or enter the LEZ sooner or later. 17 see e.g. Umweltbundesamt Vienna, 23 February

58 Service Request 6 final report Developing future objective(s) for PM2.5 Public procurement policies Public procurement, either directly by Member States or by others as a condition of the receipt of public subsidies, has been widely applied as a means of engineering the vehicle fleet. Municipal vehicle fleets and buses cover large distances in cities and can be a relevant source of air pollution. Also, they have a large share in heavy vehicles and diesel engines. In addition, public bodies serve as a role model to the private sector and should set out policies on vehicle procurement that can be widely promoted. Retrofitting existing vehicles with diesel particulate filters (DPFs) and furnishing new ones with effective filters or other clean technologies are relevant solutions which we ve rewarded in this ranking. Cities have different strategies which include retrofitting existing vehicles, acquiring new ones, reducing the fleet or investing in alternative energy sources. As with other measures, the timeline for cleaning the municipal fleet is an important aspect that we have taken into consideration. Traffic management These include measures to maximise the efficient and reliable operation of the existing road network and to minimise the impact of planned interventions on the road network, including those that have the potential to disrupt traffic flows, such as road works, which are being addressed by the London Permit Scheme among other measures. Modal shift Modal Shift Measures raise the share of public transport, reduce car use, increase cycling and walking. They encouraging smarter choices and sustainable travel by e.g. network expansion and modernisation of railway lines at city level, disabled-friendly bus stops and fleet renewal. Also introduction of pedestrian zones, improvement for cyclists, increased parking fees and cycle hire schemes are important elements. Other transport measures Other measures include inter alia promoting technological change and cleaner vehicles, provision of electrical vehicle charging points and reduction of idling periods Measures for exceedance situations where industrial, heat and power production emissions dominate Actions shown to reduce PM 2.5 emissions from industrial, heat and power production are given in Table Umweltbundesamt Vienna, 23 February 2013

59 Service Request 6 final report Developing future objective(s) for PM2.5 Table 7: Additional actions that have been demonstrated to reduce PM 2.5 emissions from stationary sources according to the US EPA. Stationary Source Actions Stationary diesel engine retrofit, rebuild or replacement, with catalysed particle filter New or upgraded emission control requirements for direct PM 2.5 emissions at stationary sources (e.g., baghouse or electrostatic precipitators; and improved monitoring methods) New or upgraded emission controls for PM 2.5 precursors at stationary sources (e.g., wet/dry scrubbers) Energy efficiency measures to reduce fuel consumption Measures to reduce fugitive dust from industrial sites NOTE: These actions are additional to those taken to meet extant legal obligations. The actions, depending on the stringency of implementation are effective in avoiding, reducing or abating emissions of PM and, in some cases, NO x ; they also tend to reduce the background emission and may assist in reducing average exposure (as measured by AEI) and NERTs. These include: Improved process design Energy efficiency measures Tightening existing emissions standards and permits as opportunity allows, by: The use of less polluting fuels (natural gas, biogas, light oils etc) Optimized facility maintenance programmes Improved combustion plants efficiency and refurbishment of equipment Establish procedures for pollution days More stringent application of existing legislation. Fostering of inspection Measures for where agricultural 18, commercial, public and residential emissions dominate Actions shown to reduce PM 2.5 emissions from agriculture, commercial, public and residential sources are given in Table 8. These actions were mapped onto measures commonly deployed in the Member States to reduce PM 10 emissions and encompass measures which reduce combustion emissions from commercial, public and residential buildings and activities. 18 Agriculture is included at here as it is usually rural and its contribution to background tends to be its most significant impact. Umweltbundesamt Vienna, 23 February

60 Service Request 6 final report Developing future objective(s) for PM2.5 Table 8: Additional actions that have been demonstrated to reduce PM 2.5 emissions from agriculture, commercial, public and residential sources according to the US EPA. Area Source Actions New open burning regulations and/or measures to minimize emissions from forestry and agricultural burning activities Smoke management programs to reduce domestic coal use Reduce emissions from woodstoves and fireplaces Regulate charbroiling/other commercial cooking operations Further reduce solvent usage or solvent substitution (particularly for organic compounds with 7 carbon atoms or more, such as toluene, xylene, and trimethyl benzene) NOTE: These actions are additional to those taken to meet extant legal obligations. These actions also reduce the background emission and may assist in reducing average exposure (as measured by AEI) and NERTs. These include: Avoiding, reducing and/or abating combustion emissions (solid and liquid fuels) Combined Heat and Power (CHP) Energy efficiency, retrofitting public housing stock. Clean air zones Small combustion plant inspection systems Additional requirements for planning consents Improved policing of or extension to smoke control zones National small combustion plant regulations are an important measure to control PM in the localised areas. For example, in the UK the Clean Air Act (CAA) regulates emissions from residential heating, commercial/institutional heating and, small industrial activity (heating and process emissions). The recent revision to the Gothenburg protocol sets national emission ceilings for PM 2.5. The contribution of small combustion activities to the new 2020 ceilings for PM 2.5 are about 20 % which indicates the importance of these activities when considering measures to address the new ceilings for PM 2.5. Part II of the CAA (Article 4) requires new non-domestic furnaces and boilers to be capable of smokeless operation and to be notified and plans approved by the Local Authority Part II of the CAA (Articles 14 to 16) includes provision for approval of chimney height for non-domestic furnaces Part III (Article 18) of the CAA allows the designation of Smoke Control Areas (SCA). Article 20 prohibits emission of smoke from building chimneys and from chimneys serving furnaces of any fixed boiler or industrial plant in an SCA. Smoke Control Area provisions have been effective in controlling emissions from domestic solid fuel combustion including significant impacts on national emissions of Benzo(a)pyrene, PM 10 and PM 2.5. PM 2.5 domestic fuel emissions are predicted to increase 5 times in smoke control areas if current authorised smokeless fuels were to be replaced with wood (AEA 2012). In Germany 19 an ordinance 20 ( 1. BImSchV ) provides for stringent emission limit values for PM (and other pollutants) for new heating systems. Limit values have also been set for existing 19 The Danish Environment ministry announced on 6 December 2012 to implement new, thighter emission limit values for stoves, Umweltbundesamt Vienna, 23 February 2013

61 Service Request 6 final report Developing future objective(s) for PM2.5 stoves and ovens, for which compliance has to be proven or a retrofitting or replacement has to be undertaken until 2024 at the latest. In addition this ordinance stipulates that operators must be advised on the proper handling of the heating systems and the solid fuels to be used. In addition, wood fuel will be checked regularly for quality in the framework of other monitoring tasks. There is anecdotal evidence that fuel or energy poverty and increase in gas and oil prices might lead to increased use of low quality solid fuel or waste for residential heating. This could result in increased levels of PM and PAH in various areas in Europe. Fuel poverty in general is defined as a situation where households cannot afford or have to use a high percentage of income to heat their homes to an adequate level (see e.g. BOUZAROVSKI BUZAR, S. 2011; BRUNNER ET AL. 2011; THOMSON, H. & SNELL, C. 2012; CASE 2012). The reasons might be low incomes, high fuel prices and/or energy-inefficient buildings (and heating systems). Improvements of building insulations and heating systems in general result in a reduction of emissions as well Measures for agriculture suitable for PM exceedance situations The reductions achievable in PM levels (particularly for PM 2.5 ) by local measures is limited due to dominant regional background concentrations, it is recommended that consideration is given to further decrease emissions by gaseous precursors (e.g. NO x, SO 2 and NH 3 ) at EU level (NEC Directive) to further decrease the regional background of PM. Also, given their rural nature, measures for agriculture have the greatest potential for influencing background concentrations NH 3. These measures include: Reduce NH 3 emissions Control agricultural burning Control dust emissions Measures to reduce NH 3 emissions are indicated inter alia in the UNECE Gothenburg protocol and supporting documents for this protocol and the IPPC Directive. Within the Nitrates Directive Member States established codes of good agricultural practice and developed specific action programmes. Possible and effective measures include those that are part of good agricultural practice, e.g. timing of manure application and low emission techniques (e.g. band spreading, subsequent incorporation of manure, slurry injection, ), reduced application of urea or treatment of exhaust air by scrubbers and biotrickling filters in pig housing. Agricultural waste burning releases PM 2.5 to the air and in the recent GAINS model agriculture accounts for 13 % of PM 2.5 emissions (IIASA 2012a, 2012b, 2012c). Projections to 2030 show that the contribution of agriculture to PM 2.5 is expected to grow as the current legislation baseline does not foresee any additional legislation in this area. The Good Agricultural and Environmental Condition (GAEC) of the Common Agricultural Policy (CAP) sets out a ban of burning of straw and stubbles in most MS. In addition some MS also ban agricultural burning under national legislation, e.g., Denmark since 1991 and England since Consequently, many national emissions inventories 21 show a decline in emissions of PM from agriculture. However, IIASA reported evidence of continued burning in many MS from remote sensing data derived from the Global Fire Emission Database (GFED 22 ) database. The GAINS model assumes a complete removal of PM 2.5 emissions following the implementation of a ban on agricultural waste burning. This measure is relatively low costs and therefore is 21 However, there is a incomplete reporting of emissions from this sector Umweltbundesamt Vienna, 23 February

62 Service Request 6 final report Developing future objective(s) for PM2.5 presented as an attractive option. If enforcement difficulties are overcome, this measure is likely to be cost effective across MS Other measures There are further measures available that are helpful to reduce PM levels on the long run or that are helpful to implement stringent measures. These measures are not source specific and include inter alia: Development of forest on open areas in and adjacent to urban centres with high PM levels. The establishment of vegetation barriers alongside busy roads and beside industrial plant. Improved transparency and communication of air quality plans with emittors (i.e. airports, large commercial organisations etc) and the public. Strategic planning tackling emissions associated with new developments Measures that mainly reduce PM 10 but hardly PM 2.5 In the time extension notifications for PM 10 a considerable number of measures were listed that aim to reducing the coarse fraction (PM ) but are of limited effectiveness for reducing PM 2.5. These are inter alia: Street sweeping: In a review study on the effectiveness of street sweeping no clear evidence was found for the reduction of PM 10 (AMATO et al. 2010). In this study the ratio of exhaust to non-exhaust vehicle emissions was named to be 1.2 for PM 10 but 4 for PM 2.5. Given the fact that street sweeping is expected to affect mostly the coarse fraction, the impact on PM 2.5 is likely to be small. Winter sanding: The PM 2.5 fraction of street wear and winter sanding particles in PM 10 is about % (KUPIAINEN et al. 2005, TERVAHATTU et al. 2006). This considerably limits the impact on PM 2.5 concentrations of measures to control winter sanding. Chemical dust suppressants: In a recent study on the effectiveness of reduction of PM 10 and PM 2.5 by applying Calcium Magnesium Acetate (CMA) on roads an effect of about 10 % for PM 10 and about 3% for PM 2.5 was found (URS 2011). The authors also concluded that further work is required to confirm these effects. Construction work: Also in the case of construction work, for mechanical generated dust the fraction of PM 2.5 in PM 10 is about 20 % (see e.g. WATSON & CHOW 2000). Therefore the effectiveness of reducing dust at construction sites is 5 times lower for PM 2.5 than for PM 10. However, this would be improved with more measures to control exhaust emissions from construction machinery and construction site traffic were put in place Overview In the following table the effectiveness of the measures described above is summarized and evaluated qualitatively for reducing various PM fractions and measurands. The actual impact is dependent on the concrete definition and implementation of the measure. The qualitative evaluation given in the table therefore reflects a subjective expert estimate for typical cases 62 Umweltbundesamt Vienna, 23 February 2013

63 Service Request 6 final report Developing future objective(s) for PM2.5 Table 9: Qualitative evaluation of the effectiveness of different measures on various PM fractions and constituents. Type of measure Measure PM fraction Comment PM 10 PM 2.5 PM UFP EC/BC low emission zone traffic Public procurement policies usually the number of vehicles affected is small. However, locally the impact can be high (e.g. roads or places with high share of public buses) traffic management +, ++ +, ++ +, ++ +, ++ +, ++ modal shift +, ++ +, ++ +, ++ +, ++ +, ++ other transport measures +, ++ 0, , + industry Avoiding, reducing, and abating emissions agriculture commercial, public, residential other NH 3 emissions agricultural burning Misc. measures e.g. forests, vegetation barriers strategic planning street sweeping, winter sanding 0, PM 10 chemical dust suppressants + 0, construction In principle, a target aim is to set policy and legislation so that the majority of pollution issues are addressed with Community wide measures, with more difficult issues being addressed via national measures. For isolated issues set in local circumstances, then local measures should be relied upon to reduce emissions in these instances, but on the whole these should not arise in the norm. The implementation of this principle, has in recent years proved difficult to deliver as Community wide measures such as the EURO standards in meeting emission standards in real world driving conditions has resulted in higher emissions that what was expected. At this point, it is difficult to predict the impact of European Community wide measures compared with national/local measures in relation to PM but it is important that we should adequately assess the uncertainties in these measures and compare with standard compliance. The uncertainties in the deliverance of Euro 6 standards have been assessed by IIASA (IIASA 2012d). While it is noted that PM impact is related to the concentrations of total PM2.5 in the air and this comprises both directly emitted particles and secondary particles (PM2.5 formed in the air by chemical reaction), NOx and NH3 are important to examine as they contribute to secondary PM2.5. The GAINS model has been used by IIASA to show that if we assume Euro VI/6 emissions calculated with COPERT 4 for PM reduction then Euro VI only delivers a 50 % improvement over Euro V. However, if the baseline NO x emissions were adjusted in each MS to account for the greater transport NOx emissions before the optimisation scenarios were run then the results as- Umweltbundesamt Vienna, 23 February

64 Service Request 6 final report Developing future objective(s) for PM2.5 suming a future Euro VI delivers a 50% improvement over Euro V and Euro 6 is the same as Euro 5. Clearly, some uncertainty remains over the real world deliverance of the Community wide measures already in place. It important that a close watching brief is maintained in this area to monitor the compliance gap, and the ability of various measures to close this gap year on year Questionnaire on air quality management for PM 2.5 reduction targets and exposure obligation In September 2012 an informal questionnaire on air quality management for the PM 2.5 reduction targets and exposure obligation was sent on behalf of the Commission to the members of the Air Quality Committee. It was aimed at national and regional authorities responsible for PM 2.5 management. The questionnaire addressed the following themes: 1. The National Exposure Reduction Target (NERT) and the Exposure Concentration Obligation (ECO) for PM 2.5 ; 2. Information on PM 2.5 projections and measures, as well as accompanying studies; 3. Suggestions by Member States for alternative approaches than those laid down in Annex XIV of the AQD. Fourteen replies were received, of which ten came from representatives of a national authority (Hungary, Ireland, Lithuania, Luxembourg, Malta, Netherlands, Norway, Poland, Spain, Sweden, United Kingdom) and three came from the three regions in Belgium. All replies have been made available to the Commission. Most respondents had not yet analysed the need of measures to achieve the NERT or ECO. Seven respondents gave suggestions about alternative concepts to reduce exposure to PM 2.5. Suggestions given by more than one respondent are: Four respondents suggested giving more attention to black carbon or combustion aerosol. Three respondents pointed out that the NERT and ECO levels are dominated by large scale pollution and should in the first place be addressed by EU-wide policies. Two respondents suggested to adopt a population weighted AEI. 4.5 Overview of current levels, projections, reduction potential and technical feasibility for attaining selected PM standards Under the service contract Monitoring and Assessment of Sectorial Implementation Actions a consortium led by IIASA has developed projections of emissions and air quality. The most relevant results in relation to the PM standards are given in recent report by IIASA (IIASA 2012e). Several scenarios are considered: a baseline scenario (current legislation CLE), the Maximum Technical Feasible Reduction (MTFR) Scenario, in which all possible technical measures, irrespective of costs, are assumed in force, and three policy scenarios in which emission reductions are assumed of low, medium and high ambition, corresponding to closure of the gap between CLE and MTFR of respectively 25%, 50% and 75%. In model calculations projections of ambient concentrations in 2020, 2025, 2030 and 2050 were done for rural as well as urban background levels in Europe. Using a scaling method for the measured concentration difference between hotspot stations and nearby urban background stations estimates could also be made of the future concentrations at hotspot stations. 64 Umweltbundesamt Vienna, 23 February 2013

65 Service Request 6 final report Developing future objective(s) for PM2.5 Table 10 shows the expected non-compliance with the current PM 10 limit values in 2030 in the various scenarios. Compared to the non-compliance of today (around 2010, 25% of the stations did not comply with the PM 10 limit values), a considerable progress towards compliance is be expected, but in all scenarios a significant number of stations are predicted to not achieve compliance: For the baseline scenario this number is of the order of 10% of the stations, which goes down to roughly 5% in the most ambitious policy scenarios. Table 10 Estimated percentage of stations in compliance with the current PM 10 limit values in The three scenario cases reflect low, medium and high ambition. The three columns indicate the likeliness of the percentages (IIASA 2012e). Scenario Percentage of stations in compliance with the current PM 10 limit values Likely Uncertain Unlikely Baseline 84% 13% 3% Low case 86% 11% 3% Mid case 88% 10% 3% High case 89% 9% 2% Maximum Technical Feasible Reduction 92% 6% 2% Other information on PM levels was obtained from the work in Task 1 of the service contract and the questionnaire for the Air Quality Committee on PM 2.5, see Table 11. Umweltbundesamt Vienna, 23 February

66 Service Request 6 final report Developing future objective(s) for PM2.5 Table 11: Maximum levels of PM 10 and PM 2.5 in and around Exceedances of limit values and ECO in bold (source: AirBase; AEI levels either from questionnaire 2004/461/EC or reply to specific questionnaire for Task 3). Self-reported data are taken from the answers to the questionnaire on PM 2.5. Member State/Country PM 10 exc. days PM 10 annual mean PM 2.5 annual mean AEI AEI self-reported NERT NERT selfreported * Austria % Belgium % 20% Bulgaria Cyprus Czech Republic Denmark % Estonia Finland % France Germany % Greece % Hungary µg/m³ 18 µg/m³ Ireland % 10% Italy Latvia % Lithuania % 10% Luxembourg % 15% Malta % Netherlands % 15% Poland µg/m³ 18 µg/m³ Portugal Romania Slovakia Slovenia % Spain % 15% Sweden % 0% * Or derived from the self-reported AEI value 4.6 Detailed assessment of possible new standards, conclusions and recommendations Options for changes The options considered for changing in the current standards, for introducing new PM standards and for simplifying the current set of standards by withdrawing one or several standards are listed below. 66 Umweltbundesamt Vienna, 23 February 2013

67 Service Request 6 final report Developing future objective(s) for PM2.5 Possible changes of the current standards Binding nature Fully binding Making the NERT binding Binding with use of the Commission s discretional power Derogations for locations where the standard cannot be met Further time extension for attainment of PM standards Streamlining the time extension procedure Derogations/exemptions for designated areas Target values Enforcing Member States to take all proportionate measures required by the NERT Complementing the limit values with a target value and enforcing that proportionate measures are taken to achieve the target value Target values for new PM fractions Alert and information thresholds Timeline, Stage 2 standards Long term objectives Non-binding health indicator Parameter Redefining the NERT as a concentration target Applying the NERT and ECO to the national contribution to AEI only Numeric values Changing the levels to be attained Smoothing the NERT table Attainment dates Harmonising attainment dates with emission legislation Long term objective Stage 2 standards or a timeline for standards Temporal aspects other than the attainment date Hourly standard Introducing a 24-hour standard for PM 2.5 Multiyear limit values Percentiles of 24-hour averages Spatial aspects Further specifying the spatial application of the limit values Defining the spatial application as properties of the standards Changing the averaging area of the AEI Statistical form Improving the relation to exposure Improving the application of the limit values to locations where people live Weighting the Average Exposure Indicator by population density Relating standards directly to actual exposure Umweltbundesamt Vienna, 23 February

68 Service Request 6 final report Developing future objective(s) for PM2.5 a. Possible standards for new PM fractions Elemental Carbon and Black Carbon Ultrafine Particles PM Other PM fractions b. Simplification of the set of PM air quality standards Withdrawing one of the PM 10 limit values Replacing both limit values for PM 10 by an equivalent or stricter limit value for PM 2.5 Replacing the limit value for PM 2.5 by an equivalent or stricter limit value for PM 10 Withdrawing the ECO while keeping the NERT Farther going simplifications Keeping a binding NERT in combination with a reduced number of PM limit values Analysis of options for change For these possibilities advantages and disadvantages of changes were systematically discussed. The purpose of the analysis was not to give final answers, but to present the most relevant considerations for decisions on changes. We attempted balancing pros and cons and to draw conclusions on desirability, but a fully objective trade-off between pros and cons of changes was not possible. Before summarising our conclusions and recommendations, we discussed some considerations that should be leading in the final decision making process. Regulatory stability and improvement of standards Based on the set of criteria set out above, we identified several possibilities for improving the PM standards. If standards are indeed changed to bring about the expected improvements, the implementation process in Member States currently still not without problems will to some extent be disturbed; a change of a standard may also reduce the effectiveness of planned or already implemented policies and measures; it may cause an extra administrative burden to Member States. In our recommendations we left the balance between the added value of improvement options and the weight of regulatory stability up to the decision making process; we only recommended considering changes. Complexity and refinement of standards Virtually all standards relate to a simplified representation of the real world. Annual mean air quality limit values apply to outdoor locations even though nobody will ever be actually exposed there for a whole year. Standards may be refined by setting different requirements for different situations. Differentiation can make standards more rational and precise, but it will usually also make the standards more complicated and difficult to understand. For standards that are only used by specialists, e.g. standards for medical equipment, complexity is more acceptable than for standards such as speed limits, which need to be understood by the general population. Air quality standards are in an intermediate position: it is not necessary for everyone to understand them, but it is important that they can be communicated and understood by the public and stakeholders participat- 68 Umweltbundesamt Vienna, 23 February 2013

69 Service Request 6 final report Developing future objective(s) for PM2.5 ing in air quality policy. The current set of PM standards is more complicated than most standards for other pollutants, which makes communication difficult. Therefore complexity should be an important consideration. Health protection and costs of attainment In our analysis projections of attainable levels by IIASA were included. We evaluated the connection between the binding nature of the standards and the level to be attained, the main determinants of the ambition in the health protection provided by the standards. We did not give recommendations on the ambition level and left this to the realm of decision making. Compliance assessment and refinement of standards There are still important differences in the assessment practice between Member States. Especially the limit value, with a high spatial resolution and to be attained everywhere, is problematic in this respect: exceedances at hotspot locations identified in one Member State may go undetected in other Member States due of differences in station siting strategies and/or modelling capabilities. The expected health protection of refinements of the standards will in practice not be gathered when the refinements are not reflected in the compliance assessment practice within Member States Changes in the PM standards proposed for consideration In the recommendations we distinguished three groups of possibilities mentioned above: 1) Optimising the existing standards; 2) Adding standards; 3) Withdrawing standards Optimising the existing standards Options for optimising the existing standards are arranged under three headings: a. Binding nature, flexibility arrangements and spatial differentiation, b. Changes in the levels to be attained, c. Refinements of a more technical nature. a. Binding nature, flexibility arrangements and spatial differentiation Air quality standards that set a fixed level to be attained everywhere, provide a minimum protection. Because PM is harmful at all levels and because the levels that can be attained vary considerably over EU, standards are desirable that drive levels down everywhere where this is possible. The local reduction potential can be taken into account by including flexibility in the binding nature of the standard or by setting different objectives for different designated areas. Flexibility options considered are: Making the NERT more binding. Enforcing Member States to take all proportionate measures The NERT is as target value a weak driver for action. To strengthen it we recommended considering making the NERT binding, by introducing an enforcement mechanism for taking proportionate measure or by making it binding with derogation possibilities. Umweltbundesamt Vienna, 23 February

70 Service Request 6 final report Developing future objective(s) for PM2.5 Derogations (possibly streamlined) of otherwise binding standards The existing time extension procedure could be re-introduced. Widespread derogations should not be foreseen however. Possibilities for streamlining the derogation procedures have been suggested. Spatial differentiation of standards Instead of ad hoc derogations on request, structural exemptions may be set for specified types of areas, e.g. cities larger than some size. Because transboundary air pollution is an important contributor to attainability problems, clear and simple physical or administrative criteria for exemption of areas do not seem feasible. The NERT, specifying different targets per Member State, has an implicit spatial differentiation but it does not take the reduction potential into account. Also for the limit values, flexibility can be achieved by derogations or spatial differentiation or, alternatively, by complementing the limit values with a target value for which taking proportionate measures is enforced. b. Changes in the level to be attained The projections of PM levels in future years and the scenarios for reduction policies developed by IIASA show that reductions of PM concentrations are possible everywhere in the EU. In certain areas the existing limit values will not be attained, even in the most ambitious scenarios. A large share of the possible reductions is due to emission reduction under EU legislation (national emission ceilings and sectoral emission standards). This is particularly the case for the projected AEI levels. The scenarios do not include all possible local measures, but it is likely that local measures cannot bring the levels much further down than the levels calculated. We did not give recommendations on changes in the levels to be attained. We recommend however considering setting (or maintaining) lower levels than those attainable everywhere, in combination with flexibility arrangements (see above). Attainment dates obviously relate to the levels to be attained. In order to convey to stakeholders and citizens the message that levels to be attained are far above healthy levels, we recommend considering setting out a timeline for PM standards. A long-term objective, such as exists already for ozone, does not seem a viable option. c. Refinements of a more technical nature The definition of the reduction objective of the NERT may be improved by smoothing the NERT table and redefining it as a target concentration. In order to reduce compliance fluctuations from year to year due to meteorological fluctuations when the PM levels are very close to the level to be attained, three-year averaging for the limit values could be considered. The number of compliance fluctuation cases is estimated to be almost halved, but this may not be a significant improvement compared to drawbacks. We considered possibilities to reduce the averaging area of the AEI, but on balance do not deem this an improvement. To improve the representativeness of the AEI for the average exposure, the concentration at each station contributing to the AEI could be weighted by the population represented by the station. We deem the pros and cons approximately in balance. The limit values could be exclusively related to locations where people live, but we do not recommend this. 70 Umweltbundesamt Vienna, 23 February 2013

71 Service Request 6 final report Developing future objective(s) for PM2.5 The spatial extent of the limit values is currently partly described in siting requirements. Some clarity may be gained by defining the spatial application as properties of the limit values Adding standards 24-hour PM 2.5 limit value In its answers, WHO has proposed regulation of short-term average concentrations (such as the 24 hour mean), in addition to the existing annual limit value for PM 2.5 and the two PM 10 limit values. The additional health protection in relation to the indirect protection provided by the overlap with existing limit values strongly depends on the level to be attained, which is not investigated here. Because a new PM 2.5 would increase the already substantial complexity of the current set of standards, it will be important to carefully balance the added protection against the drawbacks of a new 24 hour limit value for PM 2.5. New PM fractions For new PM fractions, in particular black carbon and ultrafine particles, evidence on the health impact has emerged. Because of uncertainties in attainable levels of possible standards and immaturities in methods for assessing exceedance, binding standards for these fractions are deemed premature. For black carbon synergy of air quality policy with climate change policy would best be achieved in emission legislation. For the option of target values with a weak binding nature the added value is considered insufficient to counterbalance the disadvantage of the higher complexity of the set of PM standards, but guidance on the use of black carbon as health indicator would be useful for local policy making. In anticipation of possible future standards for black, elemental or organic carbon and/or UFP we recommend requiring more extensive monitoring in order to acquire data on ambient concentrations and to improve monitoring practice for these PM fractions Withdrawing standards With health protection being the primary criterion for its recommendations, WHO is not recommending withdrawing any of the PM standards. Many stakeholders on the other hand regard the current set of standards as very complex and difficult to understand and communicate in the policy making process. Because the various PM standards overlap to a considerable extent, it was appropriate to investigate the possibility of withdrawing one of more standards without losing substantial health protection, possibly by strengthening other standards. We identified several possible options for reducing the number of PM standards. For all options the remaining set of standards need to be tightened in order to fully or approximately achieve the same level of protection against health effects given by the existing set of PM standards. In addition, these options are not in accordance with the WHO recommendations. Umweltbundesamt Vienna, 23 February

72 Service Request 6 final report Developing future objectives for heavy metals and PAHs 5 DEVELOPING FUTURE OBJECTIVES FOR HEAVY METALS AND PAHS 5.1 Key messages Heavy metals Reported exceedances of the existing target values are associated with a small number of industrial sources. There is some evidence that the existing target values are ensuring that measures are being taken to tackle these industrial exceedances by reducing emissions. There is limited detailed understanding available of the relationships between sources and ambient concentrations. There is also information missing on the assessment and concentration levels around several sources that emit high quantities of heavy metals. Resuspension of contaminated soil was shown to be a major source of cadmium in one Member State. However, no information was available on the contribution of resuspension in other areas. Contributions from resuspension could make compliance difficult in some locations even if emissions to air are largely abated. There is very little quantitative evidence available of the impact of the abatement measures that have been taken. More information on measures and their impact may become available once the existing target values come into force on 31 December 2012 and mandatory reporting by MS on measures commences. The draft answers by WHO to answers concerning current target values for heavy metals suggest not changing the provisions for arsenic and nickel. However, for cadmium strengthened evidence on health impacts and still too high input levels to agricultural soils suggest adapting the target value and/or emission legislation. Polycyclic aromatic hydrocarbons Most of the reporting exceedances are associated with domestic heating emissions. There is some evidence that the existing TV are ensuring that measures are being taken to tackle industrial exceedances by reducing emissions. There is very little quantitative evidence available of the impact of the abatement measures that have been taken. Especially, there is very little information available on measures taken to reduce emissions from domestic heating, which is the predominant source of emissions in most areas. This situation might improve in the next few years when compliance with the target value is aimed for from 2013 onwards. The detailed information required for assessing the effort for compliance, which is currently not available, suggests that the current target value approach is more appropriate than binding limit values. A reduction to a much lower value would result in very widespread exceedances across almost all of the EU, which would mean that it would be hard to target measures at the worst affected areas. 72 Umweltbundesamt Vienna, 23 February 2013

73 Service Request 6 final report Developing future objectives for heavy metals and PAHs It might be considered applying an exposure reduction approach to urban background concentrations of B(a)P in a similar way to the treatment of PM 2.5 in the AQD. This might be one way to tackle the widespread nature of exceedances of the current target value. Mercury Exposure to ambient air concentrations is not a significant contributor to human exposure to mercury. Therefore it is recommended continuing of monitoring ambient concentrations of Hg in both urban areas and industrial hotspots and continuing abatement of emissions on international level. An implementation of a target value for mercury would not result in a significant reduction of exposure to mercury. The draft answers by WHO to questions concerning mercury indicate that there is no new evidence that would impact on the air quality policy for mercury. Deposition At the present only few deposition data for heavy metals and PAH collected with the reference measurement methods is available. Available deposition data show a wide range between deposition data at industrial sites and background sites; so a different sampling strategy is needed for rural and industrial sites.as there is a considerable influence in the use of different collector types to measured deposition rates, it is recommended to gain more information on and experience with the current reference measurements methods before setting target or limit values. This gap of knowledge could be closed by additional deposition monitoring on background and industrial sites. 5.2 Context Article 8 of the DD4 states that a report has to be prepared by the Commission, which should be the basis of a possible revision of the target values for Ni, As, Cd and B(a)P as well as possible further action for mercury. This report has to be based on the latest scientific findings and technological developments. In addition, it has to take into account: Current air quality trends and projections; Scope for further emission reduction; technical feasibility, cost-effectiveness and additional health and environment protection of these reductions as well as secondary effects; Combined strategies and relationships between pollutants; Information of the public and reporting (covered by section 6) Experience in the Member States; Secondary economic benefits for the environment and health Adequacy of current sampling and suitability of B(a)P as a marker for PAH (see chapter 3); Merits for further action for Hg. The focus of the analysis lies on the 27 European Member States. Where available, data for Croatia was included. Umweltbundesamt Vienna, 23 February

74 Service Request 6 final report Developing future objectives for heavy metals and PAHs 5.3 Extent of exceedances for heavy metals Current target values of the 4 th Daughter Directive The current target values for the DD4 pollutants are shown in the table below. Table 12: Target values for arsenic, cadmium, nickel and benzo(a)pyrene (source: DD4). Pollutant Target value* in ng/m³ Arsenic 6 Cadmium 5 Nickel 20 Benzo(a)pyrene 1 * For the total content in the PM 10 fraction averaged over a calendar year These target values should not be exceeded from 31 December 2012 onwards. Member States shall take all necessary measures not entailing disproportionate costs to ensure compliance Extent of exceedances of arsenic The analysis summarized in chapter 2 has shown that in 2010 exceedances of the target value for arsenic of 6 ng/m³ occurred in five MS (Table 13). It has to be noted that no data is available for Greece and Malta as well as for Croatia. Table 13: Maximum level of arsenic in 2010, number of stations affected, name of cities (source: annual questionnaire 2004/461/EC). MS max. As level (ng/m³) # of stations name of cities, regions BE Hoboken CZ Kladno-Švermov, Stehelčeves FI Harjavalta DE Braubach PL Bydgoszcz, Nakło nad Notecią Table 14 shows the area and population affected by exceedances of the target value for arsenic. Overall the area affected is 9.8 km²; 10,550 people 23 are estimated to be exposed according to questionnaire 2004/461/EC. 23 Without PL 74 Umweltbundesamt Vienna, 23 February 2013

75 Service Request 6 final report Developing future objectives for heavy metals and PAHs Table 14: Area and population affected by exceedances of the target value for arsenic in 2010 (source: annual questionnaire 2004/461/EC). MS city area (km²) population BE Hoboken CZ Kladno-Švermov* Stehelčeves* FI Harjavalta DE Braubach PL Bydgoszcz, Nakło nad Notecią (17,971) + (2,069,575) + * both stations are located close to the city of Kladno + according to the reply to the questionnaire. Numbers provided cover whole Voivodeship; however, for several stations levels were reported that were below the target value. The station type is given as industrial in Germany, Finland and Belgium, in Poland and Czech Republic as background. Figure 5 shows a map of monitored annual mean concentrations 24 of arsenic for No modelled data is available for arsenic. Figure 5: Annual mean concentration of arsenic in 2010 in ng/m³ (source: EEA 2012). 24 According to Figure 5 one Slovakian site showed an arsenic concentration above 6 ng/m³, which was not reported in questionnaire 2004/461/EC. The site Prievidza Malonecpalska had an arsenic level of 6.4 ng/m³. If given as an integer number this means no exceedance of the target value. Umweltbundesamt Vienna, 23 February

76 Service Request 6 final report Developing future objectives for heavy metals and PAHs Extent of exceedances of cadmium The analysis summarized in chapter 2 has shown that in 2010 exceedances of the target value for Cd of 5 ng/m³ occurred in five MS (Table 15). It has to be noted that no data is available for Greece and Croatia. Table 15: Level of cadmium in 2010, number of stations affected, name of cities (source: annual questionnaire 2004/461/EC). MS max. Cd level (ng/m³) # of stations name of cities, regions BE Andenne, Beerse (2 stations) BG Kardjaly, Dolny Voden, Plovdiv FI Harjavalta FR Viviez* ES Córdoba * Prefecture Aveyron in Midi Pyrénées according to the answer to the questionnaire to the French authorities. The station type is given as industrial in Belgium, Finland, France (answer to questionnaire to French authorities) and Spain, as background and traffic (Plovdiv) in Bulgaria. Table 16 shows the area and population affected by exceedances of the target value for cadmium as given in questionnaire 2004/461/EC. Overall the area affected is about 130 km²; about 445,000 people are estimated to be exposed. For Bulgaria no information on urban background levels is available from the cities affected by exceedances. The numbers provided for area and population comprise the whole city. Therefore the number provided should be used with care and can be regarded as an upper bound. In the surroundings of the industrial facilities for which more detailed information is available, the area affected in BE, FI and FR amounts to about 8 km² where about 3,300 people are living. 76 Umweltbundesamt Vienna, 23 February 2013

77 Service Request 6 final report Developing future objectives for heavy metals and PAHs Table 16: Area and population affected by exceedances of the target value for cadmium in 2010 (source: annual questionnaire 2004/461/EC). MS city area (km²) population BE Beerse Andenne Kardjaly 31 62,970 BG Dolny Voden 2 2,000 Plovdiv ,109 FI Harjavalta 1 1,500 FR Viviez* >7 >1,400 ES Córdoba (141) + (328,547) + * according to the answer to questionnaire the numbers provided are the lower limit. + whole city of Córdoba. However, an urban background station shows Cd levels well below the target value. Figure 6 shows a map of annual mean concentrations of cadmium for 2010, based on monitoring data; Figure 7 shows model results of cadmium concentrations in air in The modelled concentrations are in most parts of Europe a factor of 10 below the target value. This indicates that there are no exceedances of the target value for cadmium on regional scale. Figure 6: Annual mean concentration of cadmium in 2010 in ng/m³ (source: EEA 2012). Umweltbundesamt Vienna, 23 February

78 Service Request 6 final report Developing future objectives for heavy metals and PAHs Figure 7: Annual mean concentration of cadmium in 2009 in ng/m³ in the regional background(source: EMEP MSC-E). A comprehensive analysis of transboundary fluxes of cadmium, mercury and lead was recently published by EMEP MSC-E (EMEP MSC-E 2012) Extent of exceedances of nickel The analysis done under Task 1 has shown that in 2010 exceedances of the target value for Ni of 20 ng/m³ occurred in four MS (Table 17). It has to be noted that no data is available for Greece and Croatia. Table 17: Level of nickel in 2010, number of stations affected, name of cities (source: annual questionnaire 2004/461/EC). MS max. Ni level (ng/m³) # of stations name of cities, regions BE Genk (2 stations) DE Krefeld ES 25 1 Santa Cruz de Tenerife FR Clermont-Ferrand 78 Umweltbundesamt Vienna, 23 February 2013

79 Service Request 6 final report Developing future objectives for heavy metals and PAHs Table 18 shows the area and population affected by exceedances of the target value for nickel. Overall the area affected is about 30 km²; about 7,200 people 25 are estimated to be exposed. Table 18: Area and population affected by exceedances of the target value for nickel in 2010 (source: annual questionnaire 2004/461/EC). MS city area (km²) population BE Genk FR Clermont-Ferrand 21 1,812 DE Krefeld 7 5,000 ES Santa Cruz de Tenerife (173) + (346,879) + + Exceedance at one site only; further monitoring sites do not show exceedances. The station type is given as industrial in Belgium, France and Germany, traffic in Spain. Figure 8 shows a map of monitored annual mean concentrations of nickel for No modelled data is available for nickel. Figure 8: Annual mean concentration of nickel in 2010 in ng/m³ (source: EEA 2012). 25 The numbers given do not include the city of Santa Cruz de Tenerife in Spain. In the questionnaire 2004/461/EC the whole city is included even though eight further monitoring sites in Santa Cruz de Tenerife show levels below the target value. Umweltbundesamt Vienna, 23 February

80 Service Request 6 final report Developing future objectives for heavy metals and PAHs N.B.: In Northern Italy a nickel concentration of 20.5 ng/m³ is given in AirBase, which was not reported in questionnaire 2004/461/EC as an exceedance. 5.4 Extent of exceedances of benzo(a)pyrene The analysis summarized in chapter 2 has shown that in 2010 exceedances of the target value for benzo(a)pyrene of 1 ng/m³ occurred in twelve MS (Table 19). It has to be noted that no data is available for Greece, Romania and Croatia. No data about the area and population affected is available for Austria, Finland and Poland. For the other countries the area amounts to about 35,500 km² and the population to 17.7 millions. This number can be compared with population affected that is derived with the help of modelling calculations by MSC-E, which provide regional background concentrations on a 50x50 km² scale (Figure 9). These model calculations can of course provide only information on regional scale. Especially in mountainous areas the model cannot reflect a possible high variability on a smaller spatial scale. In addition, the uncertainties of PAH emissions have to be considered. Nevertheless, the calculations show that even in the regional background almost 18.5 Mio people might be exposed to levels above 1.0 ng/m³ (Table 19). The area amounts to 77,500 km². When combining these two sources of information we come up with a very rough estimate of population affected of about 35.5 Mio people. The calculations of MSC-E also show that exceedances might be expected in countries for which no data or exceedances were reported such as Latvia, Portugal 26, and Romania. Furthermore, it has to be noted that the number of exceeded stations derived from AirBase is higher than that provided in questionnaire 2004/461/EC. The higher number is partly due to rounding rules applied differently in the MSs. Monitoring station types affected are mostly (sub-)urban background (134 out of 185 stations), 16 stations are labelled industrial (mostly urban) and 35 traffic (mostly urban). 26 The high B(a)P concentrations in Portugal are due to relatively high overall emissions, wherefrom 75 % stem from the sector 4F Field Burning of Agricultural Waste (APAMBIENTE 2012). However, these numbers are not correct (pers. communication Teresa Costa Pereira, Agência Portuguesa do Ambiente). Therefore also the model calculations shown are not correct for Portugal. 80 Umweltbundesamt Vienna, 23 February 2013

81 Service Request 6 final report Developing future objectives for heavy metals and PAHs Table 19: Level of benzo(a)pyrene in 2010, number of stations, area and population affected (source: annual questionnaire 2004/461/EC; EMEP MSC-E, specific questionnaire to MS). MS max. B(a)P level (ng/m³) # of stations area (km²) population population MSC-E AT unavailable unavailable no exc. BG ,866, CZ ,272 6,567, ,000 DE ,810 8,495,035 no exc. FI unavailable unavailable no exc. FR (one station) 1,030 (one station) no exc. HU ,950 2,000 IT* * 357,622* 4,175,000 LT ,940 no exc. LV ,000 PL Kraków: 327 Niepołomice: 27.4 Proszowice: ,000 10,000 6,000 4,084,000 PT ,840,000 RO ,210,000 SI ,000 no exc. UK ,976 no exc. sum ,460 17,672,491 18,494,600 * no data available for Piemonte and Lombardia + no exceedances reported in questionnaire 2004/461/EC Figure 9: Modelled annual mean B(a)P concentrations in 2009 in ng/m³ (source: MSC-E, Umweltbundesamt Vienna, 23 February

82 Service Request 6 final report Developing future objectives for heavy metals and PAHs Figure 10: Annual mean B(a)P levels in 2010 in ng/m³ (Source: EEA: Assessment of industrial facilities and related monitoring sites The European Pollutant Release and Transfer Register (E-PRTR) data for 2010 was used to assess whether the existing monitoring network covers areas close to industrial facilities showing high emissions of heavy metals and PAH. The analysis was done in three steps: 1. Identification of main economic activity type causing exceedances; 2. Identification of facilities with equal or higher emissions than those for which nearby monitoring data is available; 3. Identification of distance to nearest monitoring site. This was done with the help of a GIS program. In the following the results of this analysis is shown for As, Cd, Ni and B(a)P. It has to be noted that his analysis can only provide a first glance at areas to be looked at for several reasons: In the E-PRTR for some facilities several entries are provided for different aggregates or parts of the facility. Even though we did have a look at the sum of emissions in the surrounding (2 km diameter) of each monitoring site, some facilities might have been overlooked. The release height of the pollutants is not known. Fugitive emissions are often an important source but are hardly quantified or included. 82 Umweltbundesamt Vienna, 23 February 2013

83 Service Request 6 final report Developing future objectives for heavy metals and PAHs The coordinates given do have two digits only and are sometimes erroneous. No analysis of the actual exposure was undertaken. No information is readily available on whether an air quality assessment was undertaken by the MS. A more detailed analysis would have been beyond the scope of this study. Especially, aggregating and correcting the E-PRTR datasets require some additional effort. According to the replies to the specific questionnaire sent to MS within Task 4 metal processing plants are responsible for the exceedances of arsenic, nickel and cadmium, for nickel in addition oil refineries. Therefore the analysis of E-PRTR focused on these two types of facilities. In the case of arsenic for 12 metal processing plants emissions above 300 kg have been reported 27. Only one reported exceedance of the target value for arsenic can be related to one of these facilities. Also in the case of cadmium only one exceedance was reported nearby a facility for which considerable emissions are reported. In the case of nickel, two facilities do cause exceedances at nearby monitoring sites out of about 30 that have been analysed. One reason why no further emissions are monitored lies in the fact that simply no monitoring site is situated within a reasonable distance. However, in some cases low concentration levels are reported nearby facilities showing high emissions. High emissions of heavy metals are reported for power plants as well. Whereas the pollutants from metal processing facilities are released mostly at low height either via stacks or from fugitive sources, power plants usually have high stacks and therefore a distinct dispersion characteristics. Due to the high stacks of power plants the maximum pollutant level can be expected to occur at a distance of some km from the facility. In few cases only a monitoring station lies within this distance. For the majority of power plants no nearby station, which might be affected, could be identified. It has to be noted that the E-PRTR database does not contain detailed information about the release of the pollutants such as stack height. Nevertheless, a rough estimate indicates that at least for arsenic and Ni an exceedance of the target value cannot be excluded in a distance of about 5 km around the highest emitting power plants under certain conditions. Also in the case of B(a)P the analysis of the E-PRTR database reveals several facilities showing rather high emissions but either no nearby monitoring site or no clear influence. A detailed analysis of the reasons for the large variations in monitored concentrations on the one hand and the extent of exceedances to be expected on the other hand, goes beyond the scope of this study. 5.6 Sources of exceedances The analysis undertaken in Task 1 of this project and summarized in chapter 5.3 has shown that the extent of the exceedances and the sources for those are rather different for the heavy metals and benzo(a)pyren. Whereas for heavy metals in most cases the exceedances are limited to small areas due to emissions from individual industrial facilities, for B(a)P extensive exceedances have been observed, which were caused by different sources. In some cases exceedances of limit values for two different pollutants were caused by a single source. Therefore 27 This threshold was chosen considering the extent of exceedance for arsenic in Hoboken, Belgium, and the reported emissions. Umweltbundesamt Vienna, 23 February

84 Service Request 6 final report Developing future objectives for heavy metals and PAHs in the following chapters the sources for heavy metals emissions are analysed collectively in chapter 5.6.1, whereas B(a)P is analysed in chapter Sources causing exceedances of target values for heavy metals Information on the sources of exceedances can partly be found in questionnaire 2004/461/EC on an aggregated level. The information provided in this questionnaire is summarized in Table 20. In addition, MS affected by exceedances were asked for more detailed information with the help of individual questions. The type of industrial facility is given in Table 20 as well. In most cases non-ferrous metals or steel plants are responsible for the exceedances; in one case a refinery. 84 Umweltbundesamt Vienna, 23 February 2013

85 Service Request 6 final report Developing future objectives for heavy metals and PAHs Table 20: Exceedances of heavy metal target values in 2010, cities, sources codes and possible sources (source: annual questionnaire 2004/461/EC, reply to questionnaire to Member States). MS pollutant name of cities, regions source (2004/461/EC) + source (replies from MS) As Hoboken S3 non-ferrous metal plant Andenne S3 metal plant Ath 1 chemical plant Belgium Cd Charleroi: Lodelinsart, Dampremy 1 two steel plants Beerse S3 non-ferrous metal plant Ni Genk 2 S3 iron and steel Kardjaly S3 no information provided Bulgaria Cd Dolny Voden S3 no information provided Plovdiv S2, S5 no information provided Czech Republic As Kladno-Švermov Stehelčeves various sources iron and steel plants, coke plants, combustion plants Finland As, Cd Harjavalta S3 metal plant France Cd Ni Viviez, Midi-Pyrenees S3 battery plant, Al and Mg smelter Les Ancizes-Comps (Auvergne) S3 iron and steel plant Germany Poland Spain As Braubach S3 secondary lead smelter Ni Krefeld S3 steel plant 3 Bydgoszcz S5, S2 As Nakło nad Notecią S1, S5 Cd Córdoba S3 copper and brass plants Ni Santa Cruz de Tenerife S3 oil refinery S1: Heavily trafficked urban centre S2: Proximity to a major road S3: Local industry including power production source related S5: Domestic heating 1 concentrations above the target value 1994 to 2009 in AirBase; however, these data are not correct according to the Agence Wallonne de l Air et du Climat. The target value was exceeded only in 2008 in Ath. Information on sources provided in the answer to the specific questionnaire. 2 values in AirBase showing further exceedance in Genk are not correct according to the Belgian authorities 3 steel plant has been sold and will probably be closed. Therefore no further information could be provided by the German authorities 4 according to the reply to the specific questionnaire none of these companies are responsible for the exceedances. The main reason for the exceedances is emissions from the residential sector. The share of different sectors to emissions of arsenic, cadmium and nickel on a national level is shown in Figure 11, Figure 12 and Figure 13, respectively. Obviously, these numbers on a national scale can be completely different from the local scale. Umweltbundesamt Vienna, 23 February

86 BE BG HR CY CZ DK EE FI FR DE HU IE IT LV LT MT NL PL PT RO SK SL SE UK total Service Request 6 final report Developing future objectives for heavy metals and PAHs For arsenic, overall industrial combustion has the highest share (56 %), followed by public power plants (19 %) and small combustion (13 %). There is however, a considerable variation between MS. For cadmium, small combustion has the highest share (39 %), followed by industrial combustion (30 %) and industrial processes (15 %). As for arsenic, the numbers vary considerably between MS. As for arsenic, the sector industrial combustion contributes most to nickel emissions (45 %), followed by small combustion (24 %) and public power (18 %). Again, there are large differences between MS. 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% Q_AgriWastes N_WasteIncin I_OffRoadMob H_Shipping G_RoadRail F_Solvents E_Fugitive D_IndProcess C_SmallComb B_IndustrialComb A_PublicPower 0% Figure 11: Arsenic emissions in EU27 in 2010 (source: CEIP, webdab). 86 Umweltbundesamt Vienna, 23 February 2013

87 BE BG CY CZ DE DK EE ES FI FR HR HU IE IT LT LV MT NL PL PT RO SE SK UK total AT BE BG HR CY CZ DK EE FI FR DE HU IE IT LV LT MT NL PL PT RO SK SL ES SE UK total Service Request 6 final report Developing future objectives for heavy metals and PAHs 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% T_IntAviCruise Q_AgriWastes N_WasteIncin L_OtherWasteDisp K_CivilAviCruise J_AviLTO I_OffRoadMob H_Shipping G_RoadRail F_Solvents E_Fugitive D_IndProcess C_SmallComb B_IndustrialComb A_PublicPower Figure 12: Cadmium emissions in EU27 in 2010 (source: CEIP, webdab). 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% T_IntAviCruise R_Other Q_AgriWastes N_WasteIncin L_OtherWasteDisp K_CivilAviCruise J_AviLTO I_OffRoadMob H_Shipping G_RoadRail F_Solvents E_Fugitive D_IndProcess C_SmallComb B_IndustrialComb A_PublicPower Figure 13: Nickel emissions in EU27 in 2010 (source: CEIP, webdab). Next to actual emissions there might be a substantial contribution from resuspension by contaminated soils, which is not included in emission inventories (EMEP-MSC-E 2012a). To get more detailed information on specific sources causing the exceedances of target values for heavy metals and/or B(a)P a questionnaire was sent to MS asking specific questions on details of the sources, measures to reduce emissions resulting in compliance and costs of these measures. The results of this specific questionnaire are summarized in chapter 5.6.3, and below. Umweltbundesamt Vienna, 23 February

88 Service Request 6 final report Developing future objectives for heavy metals and PAHs Sources causing exceedances of the target value for B(a)P In contrast to heavy metals the sources causing the exceedances of the target value for B(a)P are in most cases not related to single installations. In addition, a much larger area and population are affected by the exceedances. The information provided in questionnaire 2004/461 is summarized in Table 21. Table 21: Level of benzo(a)pyrene in 2010, number of stations, area and population affected (source: annual questionnaire 2004/461/EC). MS source code description AT S5 Domestic heating BG S1, S2, S3, S5 Traffic, industry, domestic heating CZ S1, S2, S3, S4, S5, S10, S12, S15, S16, S17, S19, S21 Traffic, mining, industry, domestic heating, transboundary DE S2, S3, S5, S10 Traffic, industry, domestic heating, transboundary FI S3 Industry FR S3, S5 Industry, domestic heating HU S1, S2, S3, S5, S10, S15 Traffic, industry, domestic heating, transboundary IT* S1, S3, S5, S7 Traffic, industry, domestic heating, accidental emissions LT S5 Domestic heating PL S1, S2, S3, S5, S10, PL4 Traffic, industry, domestic heating, transboundary SI S1, S5 Traffic, domestic heating UK S3, S5 Industry, domestic heating * no data available for Piemonte and Lombardia Table 21 shows that domestic heating, industry and traffic are the three source categories named most often in the annual questionnaire 2004/461/EC. Overall emissions of B(a)P from domestic heating are cited as a contributory factor to 120 of the 154 exceedances of the target value. Emissions of this sector are responsible for about 80 % of emissions of B(a)P in Europe. This is corroborated by the emission data reported by MS (Figure 14). In all countries the sector small combustion has the largest share. Overall, small combustion is reported to contribute by 84 % to B(a)P emissions. The share of traffic is above 10% in CZ (12 %), FR (21 %) and MT (25 %). According to a report from concawe in 2005, PAH emission from road traffic mostly stems from old diesel vehicles (CONCAWE 2005). Gasoline cars with three-way catalysts and diesel vehicles equipped with after-treatment systems showed very low PAH emissions. 88 Umweltbundesamt Vienna, 23 February 2013

89 BG HR CY CZ DK EE FR DE HU IE LV LT LU MT NL PL RO SK SL SE UK total Service Request 6 final report Developing future objectives for heavy metals and PAHs 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% Other sectors G_RoadRail F_Solvents E_Fugitive D_IndProcess C_SmallComb B_IndustrialComb A_PublicPower Figure 14: Source categories of B(a)P in 2010 as reported by MS (source: CEIP, webdab). An analysis done in UK shows a clear correlation between overall emissions and median concentration despite uncertainties in both emission calculations and monitoring (Figure 15, NPL 2012a). Figure 15: Comparison of UK B(a)P estimated emissions and UK median B(a)P measured concentrations from 1990 to 2009 (source: NPL 2012a). The large reduction until 1996 came from legal restrictions to agricultural waste burning and emission reductions in aluminium production (NPL 2012a) Exceedances of B(a)P due to domestic heating As described above, domestic heating of solid fuel is the major source for exceedances of the B(a)P target value in most MS. The costs and the effectiveness of options to reduce emissions from small scale combustion sources were studied for the CAFE programme by AEA Technology in 2004 (AEAT 2004). Umweltbundesamt Vienna, 23 February

90 Service Request 6 final report Developing future objectives for heavy metals and PAHs The study suggested several options to reduce PM emissions and analysed the cost effectiveness of various policy options. For the review of the AQD IIASA conducted a study on the reduction potential for households and other small scale combustion sources (IIASA 2012). Both studies focused on PM and did not touch on B(a)P. However, a reduction of PM emissions also reduces B(a)P approximately to the same relative extent. Therefore the results of these studies can be applied to B(a)P as well. IIASA concluded that PM 2.5 emissions could substantially be reduced if Eco-design 28 standards would be implemented, which are still under discussion. Of relevance in this respect are Ecodesign standards for Solid Fuel Small Combustion Installations 29 (Lot 15) and Local room heating products 30 (Lot 20). From 2005 to 2020 emissions would decline by 38 % (current baseline: 21 %). Emission control costs amount to 4.9 billion /a in 2020 in the baseline scenario and to 8.8 billion /a in the Eco-design scenario. Table 22 shows emissions of PM 2.5 from the domestic sector in the year 2005 and for the baseline scenario and the Eco-design scenario in 2020 for those countries that reported exceedances of the B(a)P target value in 2010 (see Table 19, chapter 5.4). Table 22 indicates that in the exceeded areas in most countries a larger reduction of PM 2.5 and B(a)P has to be undertaken than on average national level. For Northern Ireland a detailed study has been undertaken on sources of B(a)P exceedances, necessary emission reductions and costs (NPL 2012a). In 2010 B(a)P levels of about 2 ng/m³ were observed; the exceedances are caused by solid fuel heating systems. The study concluded that a complete replacement of these heating systems and an enforcement of smokeless zones would far outweigh the damage costs. However, enforcement of existing smoke control areas would cost around the same amount as the damage cost and may deliver reduced B(a)P concentrations. Further studies are currently not available. As for heavy metals the target values should not be exceeded from 31 December 2012 onwards. Therefore it can be expected that further information on exceeded areas, measures and costs of this measures will become available in near future Lot 15 (Solid Fuel Small Combustion Installations): 30 Lot 20 (Local room heating products): 90 Umweltbundesamt Vienna, 23 February 2013

91 Service Request 6 final report Developing future objectives for heavy metals and PAHs Table 22: PM 2.5 emissions from the domestic sector in 2005 and 2020 in the baseline and Eco-design scenario for MS that reported exceedance of the B(a) target value in 2010 (source: IIASA 2012; AirBase, questionnaire 2004/461/EC). PM 2.5 emissions in kt B(a)P concentration baseline Eco-Design max. B(a)P level ng/m³ Austria Bulgaria Czech Rep Finland* France Germany Hungary Italy Latvia Lithuania Poland Slovenia UK * exceedance caused solely by industrial facilities according to questionnaire 2004/461/EC Exceedances of B(a)P target value due to industrial sources The Member States that have named industry to be (partly) responsible for the exceedance of the B(a)P target value were asked for specific facilities, aggregates and costs of emission reductions. According to their replies, coke ovens, sintering plants and carbon cathodes plants are the main industrial sources of B(a)P Necessary emission reductions Different installations are responsible for the exceedances of heavy metals and/or B(a)P in the different member states. MS sometimes only reported emission loads (kg emission parameter / year) without further information (total capacity,...) in the reply to the specific questionnaire. In this case a comparison with Best Available Techniques Associated Emission Levels (BAT- AEL) was not possible. For some facilities adaption of the Emission Limit Value (ELV) will be necessary to be in line with the BAT Conclusions (e.g. BAT Conclusions on Iron and Steel). In other cases BAT-AELs are reached and there is still an exceedance of the relevant target values. In these cases companies together with competent authorities are elaborating programmes or action plans to further reduce the emissions. Stack emissions are reduced to a great extent and often reach the BAT-AELs. Diffuse emissions contribute to a rather high amount to the overall emissions. They have to be further reduced. Umweltbundesamt Vienna, 23 February

92 Service Request 6 final report Developing future objectives for heavy metals and PAHs In some cases parts of plants have been closed or will be closed in the near future; therefore local authorities assume to reach compliance with the target values Technical feasibility of emission reductions The specific questionnaires and further information sent from the member states provide hardly any data on measures and costs that would result in compliance with the target values. In general the installation of filters (fabric filters; Electrostatic precipitator, ESP) is applicable to new and existing plants. The combination of emission reduction techniques depend on the flue gas characteristics. Measures to reduce diffuse emissions will vary from site to site, but are applicable to all installations. Building ventilation can be installed; house in house concepts for the reduction of diffuse emissions are available Cost of emission reduction From a lead company estimated costs for a new filter system are 1,000,000 for each installation, which amounts to 3,000,000 for the three furnaces (reply to specific questionnaire). Another plant gives information on costs for the reduction of one third of its emission of 12 Mil. (reply to specific questionnaire). The relevant BREFs, in especially the BREF Iron and Steel give some data on costs: Investment for revamping two existing ESPs to last generation electrostatic precipitators was estimated in 2002 at million for a sinter plant with a 1.4 million Nm³/h gas flow (example plants: ArcelorMittal, Fos sur Mer, France). When estimating the costs of bag filter with a flow-injection unit, it should be borne in mind that these installations are not only used for dust separation but also for reducing PCDD/F, heavy metals and acid gases such as HF, HCl and SO 2. The investment is in the range of 16 to 35/Nm³/h (for new and existing plants). Decisive cost factors are pressure drop, the waste gas flow, fabric material and filter loading. The operating cost is around /t sinter and mostly depends on the costs of supplying activated carbon and limestone, and the extra energy. It can be calculated that a dry ESP for treatment of a waste gas flow of 300,000 Nm³/h will require an investment of approximately 2 million (1996 prices) for a pelletisation plant with an annual production of 4 Mt and a drying mill waste gas flow of 300,000 Nm³/h (EUROPEAN COMMISSION 2012). A variety of measures exist to reduce diffuse emissions, general costs are depending of the kind of measure or combination of measure (all cost data from BREF Iron and Steel 2012, EUROPEAN COMMISSION 2012). 5.7 Impact on health and environment of changes to current standards of As, Cd, Ni and B(a)P For the review of the AQD and DD4, WHO is currently conducting the REVIHAAP project (WHO 2012a). This project inter alia has the objective to provide the Commission and the stakeholders with an evidence-based response to specific questions regarding health aspects of amongst others PM, As, Cd, Hg, Ni and PAH. For these heavy metals and PAH the main question is, 92 Umweltbundesamt Vienna, 23 February 2013

93 Service Request 6 final report Developing future objectives for heavy metals and PAHs whether there is any new evidence on the health effects, that would impact upon current target values. Draft results of the REVIHAAP project were published in October 2012 (WHO 2012a). Concerning arsenic WHO concluded that there is some new evidence on the cancer risk of arsenic; however, this is insufficient to impact upon the current EU target value. Also for cadmium there is new and strengthened evidence on health effects. There is strong evidence that even low level Cd exposure decreases bone mineral density and increases the risk of skeletal fractures. Cd input to agricultural soil is still larger than the output; typically half of the Cd in agricultural soil originates from air. Present levels in air still lead to an increase in soil levels. WHO concludes that this should be taken into account in the review of the DD4. The studies published on occupational epidemiology for nickel in recent year do not change the unit risk estimate substantially. Therefore it is concluded that there is no significant impact on the present target value. Evidence on the effect of nickel on cardiovascular risk is still too limited. The analysis of the exceedances of the target values for arsenic, cadmium and nickel has shown that these are confined to rather limited areas and affecting a limited number of people. The reasons for these exceedances are specific industrial installations, mostly metal processing plants, in one case an oil refinery. There is however some uncertainty whether the current monitoring network for heavy metals covers all areas at risk. There are a number of sources showing high emissions but no nearby monitoring of concentration levels. A more detailed analysis would be beyond the scope of this study. The information provided by MS as a reply to specific requests did not allow identifying in most cases the costs and the additional benefit of measures with which compliance could be achieved. However, even in those cases were detailed analysis were undertaken by MS, some ambiguities and uncertainties remain about the actual sources and possible measures. This is due to the complex configuration of the facilities concerned, the large number of emission sources and complexity of these sources, which might be a stack, fugitive or diffuse. It was noted by MSs that measures have been implemented and further measures will be implemented irrespective of whether the target values will be converted to limit values. Therefore no additional benefit would arise in these cases. A lower numerical threshold for arsenic and nickel equivalent to the lower end of the proposed levels in the Position Paper (the threshold for cadmium is already equal to the lower end), would increase the number of MS, zones and cities affected to some extent. Currently, the concentration levels of heavy metals are determined as a fraction of PM 10. A change of metric to PM 2.5 would affect the assessment of nickel concentrations to some extent, as nickel has a relative high share in the coarse fraction. Concerning PAH the draft REVIHAAP results concluded that there is some new evidence to link PAH exposure to cardiovascular endpoints. However these effects cannot be separated from that of particles. Therefore these findings cannot impact on the current target value. Nevertheless, WHO once again noted that the existing target value is associated with a lifetime cancer risk of approximately 1 x In addition, a recent analysis concluded that B(a)P is a suitable marker for PAH mixtures (DELGADO-SABORIT et al. 2011). Contrary to heavy metals exceedances of the B(a)P target value are widespread in some countries. In addition in most cases no specific industrial installation is responsible for the exceedance but domestic heating resulting in emissions of many different small sources. Umweltbundesamt Vienna, 23 February

94 Service Request 6 final report Developing future objectives for heavy metals and PAHs Similar however to heavy metals, in those cases where industrial facilities contribute to the exceedance or are responsible for it, the information on sources, measures and costs is rather sparse. A lowering of the threshold for B(a)P would have a large impact on the extent of exceedances. A threshold according to the recommendations by WHO of 0.1 ng/m³ would result in exceedances in about 90 % of the air quality zones according to the current monitoring network. The current gaps in knowledge to assess the exceedances on an European level for both heavy metals and B(a)P can be summarised as following: Assessment of concentration levels to cover relevant sources; Assessment of population and area affected; Sources of emissions; Measures to achieve compliance; Cost of these measures. 5.8 Thresholds for Hg Introduction The goal of this chapter is to analyse information of the Community Mercury Strategy 31, the UNEP Global Atmospheric Mercury Assessment 32, the LRTAP framework 33 and further source in order to present pros and cons of different concepts to reduce mercury emissions and exposure (EUROPEAN COMMISSION 2005, AMAP/UNEP 2008, UNEP 2008, 2008a, 2009, 2010, COM(2005) 20 final, COM(2010) 723 final, BIO INTELLIGENCE SERVICE 2010).. Mercury exists in different forms: most mercury is emitted to the atmosphere as gaseous elemental mercury (GEM, sometimes name total gaseous mercury, TGM) and minor amounts of reactive (or oxidized) gaseous mercury (RGM) or as particulate oxidized mercury (TPM, total particulate mercury, AMAP-UNEP 2008). Whereas GEM has a rather long lifetime around one year, RGM and TPM are much more short-lived with lifetimes in the order of hours to days. Therefore RGM and TPM are more of regional concern, whereas GEM is a global issue. Figure 16 gives an overview of mercury sources and pathways, wherefrom especially primary and secondary anthropogenic sources are of interest, but also remobilisation and re-emissions might be considered Umweltbundesamt Vienna, 23 February 2013

95 Service Request 6 final report Developing future objectives for heavy metals and PAHs Figure 16: Pathways of mercury emissions (source: UNEP 2008) Emissions, concentrations and deposition of Hg Concentration levels of Hg Monitoring of mercury is comparable scarce in Europe; in 2010 a total of about 40 measurement stations in 11 Member States were reported in questionnaire 2004/461/EC, a large proportion of these are from the United Kingdom that operates two metals monitoring networks. Figure 17 shows concentration levels of Total Gaseous Mercury (TGM) in ambient air for the year A large proportion is below 3 ng/m³, with only two higher measurements of 6.5 ng/m³ for an industrial station in Belgium, 18 ng/m³ at one station in the United Kingdom. Umweltbundesamt Vienna, 23 February

96 Belgium Finland France Ireland Lithuania Malta Poland Spain Sweden United Kingdom Hg in ng/m³ Service Request 6 final report Developing future objectives for heavy metals and PAHs Figure 17: Summary of ambient concentrations of Hg at all monitoring station types for each Member State for which data is available for 2010 (source: AirBase). Figure 18 shows modelled concentrations of Hg. The highest concentrations can be found in the Po valley, in Eastern Europe and around point sources. The concentration range is rather narrow; over large areas in Europe the levels vary only between 1.4 and 1.8 ng/m³. This range of concentrations has been found in the UNEP assessment as well (AMAP/UNEP 2008). Figure 18: Modelled annual mean Hg concentrations in 2009 in ng/m³ (source: MSC-E, 96 Umweltbundesamt Vienna, 23 February 2013

97 Hg emissions in Mg Service Request 6 final report Developing future objectives for heavy metals and PAHs Emissions of Hg The Hg emissions 34 in EU27 and Croatia decreased between 1990 and 1999 by about 40 % and by additional 25 % between 2000 and 2010 (Figure 19). It has to be noted that assessment of reported data indicate relative high uncertainty of emission estimates in a number of countries and reporting of Hg emissions might be not complete (EMEP Msc-E 2012). The highest national total emissions in 2010 are reported by Poland (18 % of overall emissions), followed by Italy and Germany (both 11 %) Hg emissions SK SI SE RO PT PL NL MT LV LU LT IT IE HU HR GR GB FR FI ES EE DK DE CZ CY BG BE AT Figure 19: Hg emissions reported to EMEP in EU27 and Croatia 2000 to 2010 in Mg (source: CEIP). In Europe the most important sources for Hg emission are power plants (34 %), industrial installations (41 %) and small scale combustion sources (10 %). Significant Hg emissions are also reported for waste incineration and shipping, see Figure For Greece, Luxembourg and Romania ( ) emissions are shown as used in EMEP models. Umweltbundesamt Vienna, 23 February

98 Service Request 6 final report Developing future objectives for heavy metals and PAHs waste incineration; 4% shipping; 4% remaining sectors; 6% industrial processes; 20% public electricity; 34% small combustion; 10% industrial combustion; 21% Figure 20: Relevant source categories for Hg emissions in 2010 (source: CEIP) Deposition of Hg Figure 21 shows the spatial distribution of Hg deposition. High levels are found in Poland, Greece, Bulgaria, BeNeLux, Germany and UK. The highest ones were calculated for Greece, followed by Poland, Czech Republic, Slovakia and Luxembourg. Figure 21: Spatial distribution of Hg deposition in 2009, g/km²/y (source: EMEP MSC-E). A detailed analysis of mercury level in fish was done in Finland, Norway and Sweden (IVL 2007, NIVA 2009). It showed that in northern Europe the mercury concentrations in pike exceed the recommended limit for human consumption of mg/kg (Figure 22). On average the mercury concentrations were 0.73 mg/kg. The environmental quality standard of 0.02 mg/kg of the Water Framework Directive is exceeded throughout these countries. 98 Umweltbundesamt Vienna, 23 February 2013

99 Service Request 6 final report Developing future objectives for heavy metals and PAHs Figure 22: Map of northern Europe showing site-specific arithmetic means of observed mercury concentrations in mg/kg in pike collected in 1965 to 2004 in 2517 lakes and rivers. The dot size indicated the number of pikes analysed (source: IVL 2007) Action to reduce Hg emissions European Union In 2005 the European Union launched the Mercury strategy 35, a comprehensive plan to reduce mercury pollution within the EU and addressing global challenges as well (EUROPEAN COMMISSION 2005). 20 specific actions have been decided in order to reach the following objectives: i. reducing mercury emissions, ii. iii. iv. reducing the entry into circulation of mercury in society by cutting supply and demand, resolving the long-term fate of mercury surpluses and societal reservoirs (in products still in use or in storage), protecting against mercury exposure, v. improving understanding of the mercury problem and its solutions and vi. supporting and promoting international action on mercury. In 2010 the Commission has reviewed the Mercury strategy by assigning a study on implementation of the strategy and a stakeholder consultation process. Besides the assessment of im Umweltbundesamt Vienna, 23 February

100 Service Request 6 final report Developing future objectives for heavy metals and PAHs plementation of the strategy, possible additional actions and further assessment of selected actions including their environmental, economic and social impacts and administrative costs were compiled and discussed. Within the annexes a compilation of EU legislation concerning mercury, key policies and best practice on European and global level, additional data on mercury emissions, mercury in energy-saving light bulbs and a screening assessment of possible additional policy actions were given. The review report, composed by Bio Intelligence Service SAS summarizes the progress of the strategy as follows (Table 23, BIO INTELLIGENCE SERVICE 2010). Table 23: Assessment of the strategy implementation (source: DG ENV, BIO INTELLIGENCE SERVICE 2010). A new Communication on the review of the Community Strategy Concerning Mercury was adopted by the Commission on 7 December Finally the European Council concluded on the Review of the Community Strategy concerning Mercury in March 2011 (COUNCIL OF THE EUROPEAN UNION 2011), reaffirming the overall goal to protect human health and the environment, highlighting the efforts undertaken so far and reiterating the need for further European and global action. On behalf of the European Commission a study on the potential to reduce mercury pollution from dental amalgam and batteries has been conducted describing environmental, economic and social impacts of different options (BIO INTELLIGENCE SERVICE 2012). Dental amalgam has been the second largest mercury use in the EU in 2007, contributing 23-25% to overall EU mercury emissions to air and 9-13% of overall EU emissions to water and will be the largest use after phasing out chlor alkali plants in It has been concluded that improving enforcement 100 Umweltbundesamt Vienna, 23 February 2013