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Erfassung Der Expositionspfade Von Per- Und Polyfluorierten Chemikalien

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Erfassung Der Expositionspfade Von Per- Und Polyfluorierten Chemikalien Environmental Research of the Federal Ministry for the Environment, Nature Conservation and Nuclear Safety UFOPLAN (Main Task): Substance Risks Project No. (FKZ) (3711 63 418) Erfassung der Expositionspfade von per- und polyfluorierten Chemikalien (PFC) durch den Gebrauch PFC-haltiger Produkte – Abschätzung des Risikos für Mensch und Umwelt Understanding the exposure pathways of per- and polyfluoralkyl substances (PFASs) via use of PFASs-containing products – risk estimation for man and environment by Thomas P. Knepper1), Tobias Frömel1), Christoph Gremmel1), Inge van Driezum1), Heike Weil1) Robin Vestergren2), Ian Cousins2) 1) Hochschule Fresenius gem. GmbH, Limburger Str. 2, D- 65510 Idstein 2) Stockholm University, Department of Applied Environmental Science (ITM), S-106 91 Stockholm, Sweden ON BEHALF OF THE FEDERAL ENVIRONMENTAL AGENCY Delivery date April, 30, 2014 Abstract The contribution of outdoor jackets as a source of per- and polyfluoroalkyl substances (PFASs) regarding the environmental and human exposure in Germany and other member states of the European Union (EU) has been investigated. Following the development of robust and validated analytical methods for 24 different PFASs, a total of five impregnating agents and 16 different jackets were analyzed. Jackets were selected depending on e.g. their origin of production, textile, price and market share. In these jackets PFASs were determined in a range between 0.03 and 719 µg/m2. In particular perfluorooctanoic acid (PFOA) was omnipresent (0.02 to 171 µg/m2), although at lower concentrations compared to the precursors of perfluoroalkyl carboxylic acids (PFCAs), namely fluorotelomer alcohols (FTOHs) (< 1 ng/m2 to 698 µg/m2). Perfluoroalkane sulfonic acids (PFSAs) and their potential precursors, such as e.g. perfluorooctane sulfonamide (FOSA), were detected at a much lower frequency with concentration up to 5 µg/m2. Environmental exposure routes of PFASs from both, newly bought and freshly impregnated jackets were studied. In particular air emission of volatile PFASs precursors, such as 8:2- and 10:2-FTOH could be quantified; however additional losses having already occurred during storing of the jackets have been postulated. Also the release of PFCAs during washing could be quantified. The detected PFOA concentrations in washing water indicated a complete release of the extractable PFOA amount. Quantification of the human exposure to PFASs stemming from outdoor jackets showed, that the highest intermediate exposure for the background population was observed for PFOA (0.054 ng kg-1 day-1). This is a factor 3-10 lower than the estimated average intake via diet. However, for populations receiving an occupational exposure in outdoor clothing stores, exposure to outdoor jackets could exceed dietary intake estimates. Estimating in the worst case scenario for Germany, a surplus in the import of approximately 80 Million PFASs-containing outdoor jackets, these jackets do contribute with an amount of 0.27 kg PFOA as one particular source among many others to the PFASs burden for man and the aquatic environment. Kurzbeschreibung Es wurde untersucht, inwieweit Outdoor Jacken zur Exposition von per- und polyfluorierten Alkylverbindungen (PFASs) in der Umwelt und dem Menschen in Deutschland und anderen EU- Mitgliedsstaaten beitragen. Nach der Entwicklung von Analyseverfahren für 24 verschiedene PFASs, wurden insgesamt fünf Imprägniermittel und 16 Jacken analysiert. Die Auswahl der Jacken erfolgte u.a. nach Herstellungsland, Material, Verkaufmenge und Preis. In den untersuchten Jacken lagen die gemessenen PFASs Konzentrationen in einem Bereich zwischen 0,03 und 719 µg/m2. Neben den in höheren Konzentrationen (< 1 ng/m2 bis 698 µg/m2) vorkommenden Fluortelomeralkoholen (FTOHs) konnte auch Perfluoroktansäure (PFOA) in allen Jacken in einem Konzentrationsbereich von 0,02 bis 171 µg/m2 detektiert werden. Perfluoralkansulfonsäuren (PFSAs) und deren Präkursoren, wie z.B. Perfluoroktansulfonamid (FOSA), wurden weniger häufig und in Konzentrationen bis zu 5 µg/m2 gemessen. Weiterhin wurde u.a. die Freisetzung von PFOA-Präkursoren, wie FTOHs, in die Luft untersucht, wobei davon ausgegangen werden kann, dass sich bereits während der Lagerung der Jacken ein Teil dieser Substanzen verflüchtigt hat. Die Quantifizierung von perfluorierten Carbonsäuren in das Waschabwasser zeigt eine vollständige Freisetzung für z.B. PFOA. Die Exposition des Menschen mit PFASs aus Outdoor Jacken wurde errechnet und mit der PFASs-Aufnahme über die Nahrung verglichen. Die höchste Belastung für Menschen wurde für PFOA (0,054 ng kg-1 Tag-1) geschätzt, und liegt damit um den Faktor 3-10 niedriger als die geschätzte durchschnittliche Aufnahme über die Nahrung. Höhere Exposition können am Arbeitsplatz in Outdoorgeschäften erreicht werden. Unter der Annahme, dass die in Deutschland im Importüberschuss eingeführten 80 Millionen Jacken alle PFASs enthalten, konnte ein PFOA–Eintrag von 0,27 kg in die Gewässer errechnet werden. Zusammenfassend konnte somit nachgewiesen werden, dass aktuell Outdoor Jacken zur Umweltbelastung von PFASs und zur Exposition des Menschen beitragen. Understanding exposure pathways of PFASs via use of PFASs-containing products - -- risk estimation for man and environment Table of Contents List of Figures List of Tables List of Abbreviations 1 Overview - Objectives of the study ..............................................................................................12 2 Introduction ...................................................................................................................................13 3 Background information regarding production and use of PFASs in textile industry, with focus on DWR textiles and impregnation agents ..........................................18 3.1 Search strategy .......................................................................................................................18 3.2 Role of PFASs in outdoor jackets ..........................................................................................18 3.3 Global production volumes of PFASs ..................................................................................21 3.3.1 Historical production volumes and use of PFOS ...........................................................21 3.3.2 Production volumes of PFCAs with focus on PFOA ......................................................22 3.3.3 Production volumes of FTOHs .........................................................................................23 3.3.4 Production volumes of fluoropolymers .........................................................................23 3.3.5 Production volumes of side-chain fluorinated polymers .............................................24 3.4 Trading and consumption of PFASs with respect to DWR textiles ..................................25 3.5 Review of PFASs concentrations in textiles ........................................................................28 3.6 Environmental emissions of PFASs related to textiles .......................................................29 3.7 Estimation of the quantity of outdoor jackets imported to Germany ............................31 3.8 Measures of the textile industry for sustainable purposes ...............................................38 3.8.1 Recycling of DWR textiles ...............................................................................................38 3.8.2 Voluntary control of PFASs related to outdoor jackets ................................................39 3.8.3 Assessment of potential PFASs emissions during the production of textiles into the atmosphere, waste water, surface water and soil in the EU production sites. ..............................................................................................................40 3.9 Production of impregnating agents and their PFASs contents ........................................42 3.10 Conclusion of literature research ........................................................................................43 4 Analysis of PFASs concentrations in outdoor jackets ...............................................................44 4.1 Materials and methods .........................................................................................................44 4.1.1 Selection of DWR jackets .................................................................................................44 4.1.2 Substances and standards ................................................................................................47 4.2 Analytical method development and quality assurance ..................................................49 4.2.1 HPLC methods ...................................................................................................................49 I Understanding exposure pathways of PFASs via use of PFASs-containing products - -- risk estimation for man and environment 4.2.2 MS/MS methods ................................................................................................................49 4.2.3 Sample preparation and extraction of PFAS-a ..............................................................50 4.2.4 Sample preparation and extraction of PFAS-n ..............................................................51 4.2.5 Quantitative method PFAS-f ............................................................................................51 4.2.6 Quantification of PFASs in the jackets analyzed ...........................................................52
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