Material cycles & hazardous chemical challenges

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1 Summer School on Sustainable Chemistry in International Cooperation 14th September 17th September 2015 at Leuphana University, Lüneburg Material cycles & hazardous chemical challenges Roland Weber POPs Environmental Consulting, Lindenfirststr 23, Schwäbisch Gmünd, Germany

2 Content of Presentation From linear to circular economy Challenges of chemicals for natural material cycles Challenges with fluorinated alkylated substances Brominated flame retardants in global e-waste plastic and other material cycles. Management of polychlorinated biphenyls (PCB) and affected material cycles of waste oils. Material cycle of paper/cardboard watch out for hazardous non-halogenated chemicals. Material cycles of waste wood food contamination Conclusions

3 Challenge: Linear Material Flow & Waste Burden Municipal waste generation & management is a key environmental problem in developing/transition countries with a large share ending in landfills. Large cost factor for municipal budgets (true external cost). Such linear economy is a waste of resources and generate climate gases!

4 From Linear to Circular Economy EU Circular Economy Strategy (Roadmap 04/2015) Bonnet (ARC+) Circular Economy, saving resources, creating jobs, Green Week Brussels June 2014

5 Material Flow Analysis Scheme: Production/Use - Waste Management - Environment System boundary Chemicals Production Imports Recycl Incineration Exports Goods Trade Use Sewage Waste Water Treatm. Landfill Soil Atmosphere Hydrosphere

6 "Life-Cycle" of Persistent Organic Pollutants (POPs) and Human Exposure Technosphere/Emissions Chlorine/Bromine/ Fluorine Production (e.g. Chlor-alkali, historical processes) Thermal/Indust. (e.g. waste incineration, cement, metal industry, industrial fires) Environmental Transport Atmosphere Exposure Routes Intergenerational Chlorine/Bromine Use (e.g. pulp & paper, water treatm., TiO 2, Magnesium etc.) Organohalogen Production (e.g. Pesticides, PCBs, PERC, PVC, BFRs, PBDE, PFCs PFOS, PFOA) Reservoirs (e.g. landfills, contaminated sites, stockpiles, soil, sediments) Products (e.g. pesticides, PCB in transformers, BFRs and PFCs in EEE, textiles, carpet, plastic, PVC, etc.) Recycled Products Land Aquatic Plants Animals/ Cattle Fish & Shellfish Inhalation Food ingestion Soil ingestion Drinking water Occupational Accidental Indoor Consumer

7 12 Principles of Green Chemistry Prevent waste Use and generate substances not/little toxic to humans and environment Preserve efficacy but reduce toxicity Use renewable resources for raw materials Catalytic reagents superior to stoichiometric reagents high atom economy : incorporate all materials used into the final product Avoid derivatization Higher energy efficiency, ambient pressure & temperature Reduce use of auxiliary substances At the end of their function, chemical products should not persist in the environment Real-time, in-process monitoring and control Minimize potential for chemical accidents by appropriate choice of substances

8 An Early Globalisation in 1960s/70s: Contamination by Persistent Organic Pollutants! Discovery 1960s/70s: chlorinated chemicals which did not degrade in environment (persistent) were found to cause local disturbance of ecosystems including extinction of birds, fishes, reptiles. Discovery 1990s: Global pollution by POPs The dirty dozen PCDD PCDF PCBs DDT Aldrin Chlordane Dieldrin Endrin Persistent Organic Pollutants Persistent in environment & in organism/body Toxic to humans/biota Mobile in the environment HCB Heptachlor Toxaphene Mirex Late lessions from early warnings the precautionary principle

9 Persistent Organic Pollutants (POPs) Environmental/Transboundary Movement Persistent Organic Pollutants (e.g. PCB, Dioxins, POPs-Pesticides) Grashopper Effect 1. Evaporation 2. Atmospheric movement 3. Deposition/condensation Long range transport Travel the globe and accumulate in colder region including the contamination of the Arctic region.

10 POPs Environmental/Transboundary Movement Contamination of the Arctic LRT: Accumulation in the arctic (arctic population eats fatty food) High levels of contaminants in humans and human milk High cancer rates Girl/boy ratio of new born is more than 1 (Similar effect Seveso). These people have not used these chemicals but are contaminated from the production use and sale in industrial countries. Source: Guardian 12 Sep

11 POPs Environmental/Transboundary Movement Contamination of the Arctic LRT: Accumulation in the arctic (population Greenland, Alaska etc.). This global pollution and the inherent injustice can only be addressed by an international/global approach (Convention/MEA) Film Silent Snow (Jan van den Berg):

12 PCDD/F, PCB (&other endocrine disruptors) particular problematic during human development (lowest dose response conc.). Top of the Foodchain: Women accumulate POPs during their life and pass them to the baby during pregnancy and by breast milk -Still best to use mothers milk the first 6 months! (WHO)

13 Source: WHO/Malisch R (2003) PCDD/PCDF und PCB (WHO TEQ) in Mothers milk (3rd WHO Study) Still mothers milk is the best nutrition first 6 months (WHO)! blob=publicationfile PCB- + Dioxin-TEQ content at which the TDI of a baby is exceeded.

14 Time Trend of old & new POPs in Europe Time trend of PCB, DDT and PBDE in mothers milk in Sweden.

15 Thomas Max Müller/pixelio.de Lupo/pixelio.de Rose Eckstein/pixelio.de Floentine/pixelio.de Challenge of contamination of large material cycles: I) Food/food chain Semivolatile persistent chemicals (e.g. PFOS, PCBs; dioxin, mercury) accumulate in soils and sediments. From these matrices they are taken up by biota including food animals (chicken, beef, sheep, fish). In the Netherlands more than 50% of home produced eggs were found above the dioxin EU limits for eggs (Hoogenboom et al. 2015). Cattle grazing in flood plain areas of rivers often have elevated Dioxins or PCB levels sometimes above regulatory limits. Fishes in several German rivers are above EU environmental quality norms for Dioxin/PCB and/or PBDE recently introduced.

16 Challenge of Contamination of Large Material Cycles: I) Food/food Chain: Dioxin & PCB Pollution Baltic Sea The Baltic Sea is among the marine areas most heavily polluted by dioxins, PCBs and related compounds. Six decades contamination has resulted in Dioxin/PCB levels in fish above the EU limit for fish consumption Sweden and Finland have exemptions to market fish above EU Dioxin limits in their country with respective risk-communication to their population. The Baltic Sea is one example of the vulnerability of the open sea towards chemical & waste release Also the pollution of the Sea can only be controlled and managed by cooperation of the countries bordering the respective sea.

17 Human Background Exposure old POPs Human Dioxin exposure routes U.S.A. - POPs are ubiqitaneous in fatty food - Bioaccumulate in top predators - Intake depends on lifestyle Pork Inhalation Smoking Beef 16% Cheese/butter 12% Misc. 25% 19% Milk Poultry & eggs Fish

18 18 Life-Cycle of PFOS, related substances and PFAS Activity PFC Production (e.g. PFOS, PFXS, PFOA, PFXA PFtelomerealkohole etc.) PFC Use (e.g. production teflon, carpet, paper, use AFFF, Chromium plating, photo resist,) Emission Sources Thermal? (e.g. incineration, metal industry, industrial fires) Reservoirs (landfills, contaminated sites, stockpiles sludges, soils, sediments) Products (e.g. AFFF, carpet, leather, impregnation spray, textiles, paper ) Environmental Transport Atmosphere Land Aquatic Plants Animals/ Cattle Fish & Shellfish Exposure Routes Intergenerational Inhalation Food ingestion Occupational Drinking Water Accidental Indoor (dust, air)

19 Challenge of contamination of large material cycles: II) Water Chemical contamination of the water cycle is a threat to drinking water supply (relevance for SDG 6 on water). Emerging water pollutants are fluorinated alkylated substances (PFAS) used for surface treatment (textiles; furniture, carpets, paper) and industrial applications (fire fighting foam; metal plating). Many PFAS are highly water soluble, extremely persistent and some of them are bioaccumulative. Challenge and high cost to remove PFAS from water. Sweden is one of first countries monitoring their water reservoirs finding challenges with PFOS/PFAS contamination.

20 20 Challenge of contamination of large material cycles: II) Water: PFOS/PFAS levels North Sea RIVM Institute: Calculation of a maximum permissible PFOS conc. (MPC) for surface water: 0.65 ng/l PFOS and PFOA levels Rhine approx. 10 ng/l PFOS levels close to coast 2 to 4 ng/l PFOA/PFOA levels in open sea around 0.1 to 0.5 ng/l Theobald et al. ESPR 18: (2011).

21 21 Challenge of contamination of large material cycles: II) Water: PFOS/PFOA contamination of Oceans t PFOS reached the oceans approx. 99% of the 96000* t on their way Paul et al ES&T 43, (2009) (* t production waste) Yamashita et al. Chemosphere 70 (2008)

22 22 Challenge of contamination of large material cycles: II) Water: PFOS/PFOA contamination of Oceans Global PFAS long range transport via the ocean current t PFOS reached the oceans approx. 99% of the 96000* t on their way Paul et al ES&T 43, (2009) (* t production waste) Yamashita et al. Chemosphere 70 (2008)

23 23 Challenge of contamination of large material cycles: II) Water - Food chain Contamination and temporal trends of Stranded Melon-headed Whales for PCBs, DDT (decreasing) and of PFOS and PBDEs (increasing). Concentration (ng/g) PCBs DDTs PBDEs PFAS PFOS ** ** ** * :1982 :2001 : PFCs levels are in ng/g wet wt; PBDEs and organochlorine levels are in ng/g lipid wt *p<0.05; **p<0.01 Takaghashi S; Presentation; NIES Conference, Kyoto Oct ; PFC data cited from Hart et al. (2008)

24 24 Life-Cycle of PFOS, related substances and PFAS Activity PFC Production (e.g. PFOS, PFXS, PFOA, PFXA PFtelomerealkohole etc.) PFC Use (e.g. production teflon, carpet, paper, use AFFF, Chromium plating, photo resist,) Emission Sources Thermal? (e.g. incineration, metal industry, industrial fires) Reservoirs (landfills, contaminated sites, stockpiles sludges, soils, sediments) Products (e.g. AFFF, carpet, leather, impregnation spray, textiles, paper ) Recycled Products Environmental Transport Atmosphere Land Sewage Sludge Aquatic Plants Animals/ Cattle Fish & Shellfish Exposure Routes Intergenerational Inhalation Food ingestion Occupational Drinking Water Accidental Indoor (dust, air)

25 Challenge of contamination of large material cycles: III) Sewage Sludge To remove chemicals and other pollutants from waste water, sewage treatment plants are increasingly built also in developing countries. Sewage treatment plants transfer pollutants (POPs, heavy metals, pharmaceuticals) from the water phase to the sewage sludge. Several industrial countries do not use sewage sludge on agriculture or other soils but manage pollutants by incineration or disposal. However loss of nutrients including phosphorous which is a key resource for fertilizing and feeding the world with future challenge. Persistence is a key criteria of a chemical to threaten environmental media and natural material cycles. If a chemical degrades within days/weeks under environmental conditions (in sediment, soils, water) it does not accumulate in these cycles.

26 Brominated Flame Retardants in material cycles challenge of phase out. 26 Brominated flame retardants were/are applied since 1970s in large material flows (polymers in EEE, vehicles, construction, furniture, textiles) to reduce the ignitability. The first brominated flame retardants were listed in the Stockholm Convention for global phase out (e.g. PBDEs; HBCD, HBB).

27 Long range transport via waste & recycling flows

28 Material flows and stocks of WEEE plastic in Nigeria in major WEEE categories( ) Flows for 2000 to 2010 and for the stocks (in use & landfill/dump) for 2010 ( ) Open burning/ Source: Babayemi et al. 2014; Env Sci Pollut Res. DOI: /s

29 Substance flows/stocks PBDE of WEEE plastic Nigeria in major WEEE categories( ) Flows for 2000 to 2010 and for the stocks (in use & landfill/dump) for 2010 Open burning/ Source: Babayemi et al. 2014; Env Sci Pollut Res. DOI: /s

30 Global Comparison of PBDEs in Human Milk PBDEs in human milk: Comparison with some other regions/countries BDE-47 BDE-99 BDE-100 BDE-153 PBDEs (pg/g lipid wt) E-waste recycling site: Taizhou Control site: Lin an city, Hangzhou USA Taizhou, China Canada Japan Faroe Island UK Sweden Malaysia Philippines Korea Cambodia Indonesia Hangzhou, China Vietnam India Russia (Buryatia) Tsydenova, Tanabe et al., Env. Poll Region/country

31 31 Brominated Flame Retardants in material cycles challenge of PBDEs PBDE were listed in the Stockholm Convention in 2009 for phase-out. Some PBDE containing material cycles (e.g. WEEE plastic) are recycled and a restriction of recycling of PBDE containing materials might have resulted in the stop of large polymer recycling activities. Therefore in the Stockholm Convention listing an exemption was included for recycling of PBDE containing materials within a frame.

32 Material cycle c-octabde containing articles

33 PBDE/BFR Contamination of Recycled Plastic? What is the flow of PBDE/BFR in recycled materials? What articles are contaminated? What are risks to human and the environment? PBDE in children toys China (Chen et al, ES&T 43, 4200, 2009) Prof. Diamond with her PBDE Add. & Contam. in thermo- salad servers (PBDE&Pb) cup Samsonek& Puype (2013) Food The recycling flow of PBDE/BFR containing plastic seems largely uncontrolled No LCM. Need improvement and control!. Recommendation SC: Separation of POP-PBDE materials.

34 Material flow c-pentabde containing articles?

35 Assessment of Possible Health and Environmental Impacts of Recycling Articles containing PBDEs. Recycling of PBDE containing PUF to carpet padding (mainly in the US):

36 PBDE in serum lipid (ng/g) Assessment of Possible Health and Environmental Impact: Recycling of Polyurethane Foam & Human Exposure (US) POP-PBDE levels in workers recycling Polyurethane Foam PUR Foam recyclers Source: Stapleton et al. ES&T 42, 3453 (2008) Carpet installers Control (Spouse)

37 Emission Sources Chlorine/Bromine/ Fluorine Production (e.g. Chlor-alkali, historical processes) "Life-Cycle" of POPs/PTS and Human Exposure Thermal/Indust. (e.g. waste incineration, cement, metal industry, industrial fires) Environmental Transport Atmosphere Exposure Routes Intergenerational Chlorine/Bromine Use (e.g. pulp & paper, water treatm., TiO 2, Magnesium etc.) Organohalogen Production (e.g. Pesticides, PCBs, PERC, PVC, BFRs, PBDE, PFCs PFOS, PFOA) Reservoirs (e.g. landfills, contaminated sites, stockpiles, soil, sediments) Products (e.g. pesticides, PCB in transformers, BFRs and PFCs in EEE, textiles, carpet, plastic, PVC, etc.) Recycled Products Land Aquatic Plants Animals/ Cattle Fish & Shellfish Inhalation Food ingestion Soil ingestion Drinking water Occupational Accidental Indoor Consumer

38 Polychlorinated Biphenyls (PCBs) Challenges in material Cycles Polychlorinated biphenyls have been used in a wide range of closed and open applications. Closed applications (transformer oils, capacitors, hydraulic oils). Open applications (e.g. sealants, paints, cutting oils). The inventory and management of PCB equipment and oils have been found highly demanding in respect to time and resources. Approx. 1.3 million tonnes of PCB have been produced in history. A recent survey of global PCB inventories and management by UNEP revealed that the stockpiles of PCB contaminated oil and equipment are estimated to c. 9.3 million tonnes (UNEP 2015).

39 Polychlorinated Biphenyls (PCBs) Challenges in Material Cycles Waste oils is an large material and recycling flow including e.g. used transformer oils, lubricant oils, hydraulic oils, cutting oils. It has been discovered and documented in Sri Lanka that PCB oil from transformers going out of the grid are frequently reused by small companies to fill or refill other transformers. Furthermore the waste oil is used for the production of grease and for underbody corrosion protection of cars. In Ghana and Nigeria PCB containing waste oils were reported to be partly reused in creams or pomade. This demonstrates that PCB oils in developing countries are recycled into open applications with associated releases and human exposure.

40 Material Cycles of PCB waste oils Challenges in industrial countries: Food scandals Irish pork-crises (2008): Waste oil containing PCBs were used to dry animal feed in Ireland which was used then as commercial feed for pork and beef. Concentrations of PCDD/F and PCBs, discovered in pork at levels that were between 80 and 200 times the recommended EU limits. On 6 December 2008, the Food Safety Authority of Ireland ordered the recall and destruction of all Irish pork products dating back to 1. September. Financial damage was approximately 120 million EURO. Ref. : 1) Marnane (2012) J. Environ. Monit., 14, ) (access ).

41 Material Cycles of PCB waste oils Challenges in industrial countries: Food scandals Dioxin/PCB scandal Belgium (1999) Ca. 25 liter PCB oil were disposed in the wrong collection box for food fat/oil and mixed with 107 t fat for animal feed. Chicken eggs, meat from chicken, pork and beef were found in Belgium several hundred times above today s EU food limits. 446 poultry farms, 746 pig and 393 cattle farms impacted. 20,000 t poultry, 6,000 t pigs, 400 t cattle, million eggs (were destroyed/combusted). 1 billion US$ direct costs for Belgium food production. Ref: Fiedler et al. (2000) Study on behalf of the EU Commission, Sep Material Cycle Management: In the EU it is prohibited that industrial waste oils and waste food fats are managed within the same company!

42 Chlorinated paraffines - PBT alternatives for PCBs Production of PCBs stopped in 1980s and alternative substances are used. Chlorinated paraffines have substituted PCBs in a range of applications. (e.g. cutting oils, paints, sealants; flame retardants). Production increased by 1000% in recent decade. Today > 1 mio t/a primarily China & India (approx, total historic PCB production). Food oils in China with high ppb levels CPs (Takasuga et al. 2012). Sewage sludge contaminated in high ppm range (Switzerland). Global chlorinated paraffin-contamination of human milk at levels comparable or higher than PCBs! (Malisch R; Plenary Dioxin 2013).

43 Material Cycle of waste wood Wood was/is (partly) treated with PCP and other hazardous chemicals (PCBs; heavy metals; pesticides). PCP treated wood containing dioxins has been recycled as saw mill dust to a feed additive and contaminated chicken (Llerena et al. 2003). PCP treated waste wood has been recycled for bedding of chicken and resulted in dioxin contamination of eggs (Brambilla et al, 2010). PCB and lead painted wood used as animal bedding resulted in the contamination of chicken and chicken eggs. PCP containing waste wood used for drying feed resulted in dioxin contamination of feed and food above the EU limit. Waste wood has several exposure pathways to lifestock. A range of pollutants (POPs, heavy metals, others?) used for treatment of wood is problematic for recycling Move to wood preservation and to paints that do allow safe recycling!

44 Material Cycle of paper and cardboard Also the recycling of cardboard can lead to human exposure due to some sensitive uses in particular food packaging. Recycled cardboard contains mineral oils from solvents for inks in newspaper printing and other sources ( mg/kg incl % aromatic compounds). When used as packaging material for pasta and rice the food can become contaminated (up to 19 mg/kg). (BfR Stellungnahme Nr. 008/2010) There are more problematic chemicals and chemical groups used on paper which are transferred by recycling in new paper/card board products (e.g. PFOS/PFAS, BFRs; unintentional POPs (PCB; HCB) in pigments.

45 Conclusions Due to the shortage/finiteness of resources, society has to move towards a cycle economy with close(r) material cycles (EU strategy). Hazardous chemicals are a challenge and threat for cycle economy since materials are partly/often recycled into more sensitive uses. Challenge to control material flows the price determines the routes. Today material cycles are often global with (major) recycling taking place in developing/transition countries and challenges of control. Some of the material flows are closely linked to food and feed and can lead to direct exposure of humans. Some recycling materials are recycled into sensitive use areas and can also lead to human exposure via direct contact (e.g. kitchen tools; toys) or contamination of the indoor environment.

46 Multi-R approach for moving towards cycle economy Therefore substitution of hazardous chemical by sustainable chemicals in the (re-)design phase. Substitution of hazardous by sustainable chemicals Thank you for your attention Bonnet (ARC+) Circular Economy, saving resources, creating jobs, Green Week Brussels June 2014

47 Source: Vieth et al., Organohalogen Compounds Vol. 73, (2011) Jahr Dioxin/dl-PCB (TEQ) in German Breast Milk Die Dioxin Humanmilk contamination in Germany has significantly reduced the last 20 years by approx. 75%. However it will probably take more than 100 years until babies will be exposed below the TDI (PCB+Dioxin). Still mother milk is the best nutrition for a baby! blob=publicationfile PCB- + Dioxin-TEQ content at which the TDI of a baby is exceeded.

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