ANTHROPOGENIC EMISSIONS AND AIR QUALITY: ASSESSING THE EFFECT OF THE STANDARD NOMENCLATURE FOR AIR POLLUTION (SNAP) CATEGORIES OVER EUROPE

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1 ANTHROPOGENIC EMISSIONS AND AIR QUALITY: ASSESSING THE EFFECT OF THE STANDARD NOMENCLATURE FOR AIR POLLUTION (SNAP) CATEGORIES OVER EUROPE E. Tagaris Environmental Research Laboratory, NCSR Demokritos, Athens, Greece R.E.P. Sotiropoulou Department of Mechanical Engineering, University of Western Macedonia, Kozani, Greece Environmental Research Laboratory, NCSR Demokritos, Athens, Greece N. Gounaris, S. Andronopoulos, D. Vlachogiannis Environmental Research Laboratory, NCSR Demokritos, Athens, Greece ABSTRACT The objective of this study is to estimate the contribution of different anthropogenic emission sources on ozone mixing ratios and PM 2.5 concentrations over Europe using the EPA s Models-3 regional air quality system and the TNO anthropogenic emissions for 2006 classified into ten (10) different SNAP categories. Road transport category, which is mainly responsible for the NOx emissions, is estimated to have the major impact on Max8hrO 3 mixing ratio for July 2006 suggesting an increase by 6.8% on average over Europe, while locally it is more than 20%. Power generation category is estimated to have the major impact on PM 2.5 concentrations since it is the major source of SO 2 emissions, suggesting and increase by 22.9% on average over Europe, while locally it is more than 60%. However, agriculture category is contribute significantly on PM 2.5 concentrations, since agriculture activities are the major source of NH 3 emissions, suggesting an increased by 16.1% on average over Europe, while in regions with elevated NH 3 emissions the increase is up to 40%. INTRODUCTION Air pollution is a major environmental problem due to its known or suspected harmful effects on human health and the environment (e.g., Karnosky et al., 2007; Raaschou-Nielsen et al., 2013). Although air quality management strategies have been applied over recent years to reduce atmospheric pollutant concentrations, ozone and particulate matter pollution are still an issue. Anthropogenic, natural and biogenic emissions contribute to atmospheric pollution. While natural and biogenic emissions having an important role in regulating the atmospheric composition (e.g., over 90% of the total Volatile Organic Compounds (VOCs) entering the atmosphere are biogenic (Greenberg et al. 1999) anthropogenic emissions are the source of air quality degradation (Sienfeld and Pandis, 2006). Since only the anthropogenic part can be influenced by abatement measures, assessing the effect of different anthropogenic emission sources on gaseous and particle concentrations is very important for more effective adaptation and implementation guidelines in air quality planning. Anthropogenic emission sources have been classified into different activities according to the Standard Nomenclature for Air Pollution (SNAP). Ten (10) SNAP categories are used by the European Monitoring and Evaluation Programme (EMEP) ( and the Netherlands Organization for Applied Scientific Research (TNO) (Kuenen et al., 2011). The objective of this study is to assess the impact of each SNAP category on ozone mixing ratios and PM 2.5 concentrations over Europe and quantify their relative importance in air quality degradation. Results will contribute to an integrated assessmnet for air quality management in Europe since air pollutants released in one country can be transported in the atmosphere over thousands of kilometers affecting the air quality of other countries. METHODS Following the same methodology as described in details by Tagaris et al. (2013), and summarized below, we use the Penn State/NCAR Mesoscale Model (MM5) (Grell et al., 1994), TNO emissions (Kuenen et al., 2011) and the Community Multiscale Air Quality model (CMAQ) (Byun et al., 2006; Foley et al., 2010) to simulate air quality. Meteorology Vautard et al. (2012) have provided the meteorological fields in the framework of the AQMEII exercise ( using the Penn State/NCAR Mesoscale Model (MM5) (Grell et al., 1994). The Meteorology Chemistry Interface Processor (MCIP) (Byun et al., 1999) is used to convert MM5 output to the emissions and air quality models compatible format.

2 Emissions Gridded anthropogenic emissions for the year 2006 over Europe are provided by TNO at a degree resolution (Kuenen et al., 2011). The available data include annual total emissions of CH 4, CO, NH 3, NMVOC, NO X, PM 10, PM 2.5, and SO 2 for both area and point sources classified in the following ten (10) SNAP categories: (1) power generation, (2) residential-commercial and other combustion, (3) industrial combustion, (4) industrial processes, (5) extraction distribution of fossil fuels, (6) solvent use, (7) road transport, (8) other mobile sources, (9) waste treatment and disposal, (10) agriculture. Emissions are processed by the Sparse Matrix Operator Kernel Emissions (SMOKE v2.6) modeling system ( to convert their resolution to the resolution needed by the air quality model using monthly, weekly, and hourly time profiles provided by TNO (TNO, 2011). The Biogenic Emission Inventory System, version 3 (BEIS3) is used for processing biogenic source emissions. An extensive analysis and discussion of biogenic emissions and their impact on air quality over Europe can be found elsewhere (Tagaris et al., 2014). Air quality modeling The Community Multiscale Air Quality (CMAQ) v4.7 Modeling System (Byun et al., 2006; Foley et al., 2010) with the Carbon Bond mechanism (CB05) (Yarwood et al., 2005) is used here for the regional air quality modeling over Europe at 35km 35km spatial resolution (Figure 1). Figure 1: Modeling domain A simulation where all SNAP categories are included is defined as the base case simulation. In order to assess the impact of each SNAP category on ozone mixing ratios and PM 2.5 concentrations ten (10) sets of simulations are performed. In each simulation emissions from one SNAP category over the European land is excluded. The role of the emissions of a SNAP category is computed as the difference between the base case and the simulation without this emissions category. The simulations are performed for July 2006 using a spin up time of 10 days (i.e. June, 21 30). RESULTS AND DISCUSSION Road transport (SNAP 7) is the major source of NOx and CO emissions over the European land in July 2006 contributing about 42% and 50 % of the total NOx and CO emissions, respectively. Power generation (SNAP 1) is the major source of SO 2 emissions (about 66%) while agricultural activities (SNAP 10) are dominant in NH 3 emissions (about 93%). Solvent use (SNAP 6) is the major source of anthropogenic NMVOC emissions (about 41%) while industrial sources (SNAP 4) emit the highest particles amount (about 24% for primary PM 2.5 and 21% for primary PM 10). Since an extensive evaluation and discussion of the base line air quality predictions has been presented by Tagaris et al., 2013 we focus, here, on the impact of each SNAP category on ozone mixing ratios and PM 2.5 concentrations. SNAP 7 (road transport) is estimated to have the major impact on Max8hrO 3 mixing ratio for July 2006 (Figure 3) since ozone is formed from the photochemical oxidation of VOCs in the presence of nitrogen oxides, and road transport is mainly responsible for the NOx emissions (Figure 2). Max8hrO 3 mixing ratio is increased by 6.8% on average over Europe when emissions from SNAP 7 are included. However, an

3 increase more than 10% is simulated over most of Europe while locally (i.e., northern Italy and southern Germany) it is more than 20%. Ranking the importance of the rest of the SNAP categories on Max8hrO 3 mixing ratio, an increase by 2.9%, 2.1%, 1.7% on average over Europe is simulated when emissions from SNAP 8 (other mobile sources), SNAP 1 (power generation) and SNAP 3 (industrial combustion), respectively, are included. However, the increase could be a little bit higher than 10%, locally. A minor impact is simulated for the rest of the SNAP categories since Max8hrO 3 mixing ratio is simulated to increase up to 0.5% on average over Europe (locally up to 4%) when emissions from each of these SNAP categories are included. Figure 2: Contribution of each SNAP category to the pollutants emitted over the European land in July 2006 Atmospheric SO 2 is oxidized to sulfuric acid which reacts with ammonia to form ammonium sulfate, while gas-phase NO X oxidizes to nitric acid which reacts with ammonia to form ammonium nitrate. Therefore, SNAP 1 (power generation) is estimated to have the major impact on PM 2.5 concentrations for July 2006 (Figure 4), since power generation is the major source of the emitted SO 2 (Figure 2). PM 2.5 concentration is increased by 22.9% on average over Europe when emissions from SNAP 1 are included. However, an increase more than 40% is simulated over most of Europe while locally in southeastern Europe it is more than 60%. SNAP 10 (agriculture) is also playing an important role on PM 2.5 concentrations, since agriculture is the major source of NH 3 emissions. It is simulated an increase of 16.1% on average over Europe when emissions from SNAP 10 are included, while in regions with elevated NH 3 emissions (e.g, Belgium, the Netherlands, and northern Italy), the increase is up to 40%. Ranking the importance of the rest of the SNAP categories on PM 2.5 concentrations: SNAP 3 (industrial combustion) contribute 18% and 13% of the total SO 2 and NO X emissions, respectively; SNAP 7 (road transport) contribute 42% of the total NO X emissions; SNAP 4 (industrial processes) contribute 24% of primary PM 2.5 emissions; SNAP 8 (other mobile sources) contribute 20% of the total NO X emissions. Therefore, an increase by 8.9%, 8.6%, 7.3%, 7.1% on average over Europe is simulated when emissions from SNAP 3, SNAP 7, SNAP 4 and SNAP 8, respectively, are included. A minor impact is simulated for the rest of the SNAP categories (increase up to 3% on average over Europe when emissions from each of these SNAP categories are included), while the inclusion of SNAP 6 (solvent use) leads to a minor decrease (up to 1.2%) on PM 2.5 concentrations, locally. SNAP 6 is mainly responsible for anthropogenic NMVOC emissions (41% of the total anthropogenic NMVOCs) and the inclusion of this category results in a reduction of OH, slowing down the gas phase formation of sulfate (through SO 2 oxidation).

4 MIXING RATIO SNAP 1 SNAP 2 SNAP 3 SNAP 4 SNAP 5 SNAP 6 SNAP 7 SNAP 8 SNAP 9 SNAP 10 Figure 3: Daily average Max8hrO 3 mixing ratio for July 2006 and the related impact of each SNAP category

5 CONCENTRATION SNAP 1 SNAP 2 SNAP 3 SNAP 4 SNAP 6 SNAP 7 SNAP 5 SNAP 8 SNAP 9 SNAP 10 Figure 4: Daily average PM 2.5 concentration for July 2006 and the related impact of each SNAP category

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