A global atmospheric chemistry model for the fate and transport of PFCAs and their precursors
Open accessAbstract
Perfluorocarboxylic acids (PFCAs) are environmental contaminants that are highly persistent, and many are bio-accumulative and have been detected along with their atmospheric precursors far from emission sources. The overall importance of precursor emissions as an indirect source of PFCAs to the environment is uncertain. Previous studies have estimated the atmospheric source of PFCAs using models and degradation pathways of differing complexities, leading to quantitatively different results. We present results from simulations of atmospheric PFCA formation and fate using the chemical transport model GEOS-Chem. We simulate the most up-to-date chemistry available to our knowledge for the degradation of the precursors fluorotelomer alcohol (FTOH), fluorotelomer olefin (FTO), and fluorotelomer iodide (FTI), as well as the deposition and transport of the precursors, intermediates and end-products of the formation chemistry. We calculate yields of C3-C13 PFCAs formed from 4 : 2 to 12 : 2 fluorotelomer precursors and their deposition to the surface. We find that the ratio of long-chain to short-chain PFCAs increases strongly with distance from source regions. We compare our model results to remote deposition measurements and mid-latitude rainwater measurements. The model captures the observed relationship between rainwater abundance and PFCA chain length, as well as the average deposition rates at mid-latitude and Arctic sites, but underestimates the deposition of PFDoA, PFDA, and TFA at mid-latitudes and PFNA at the Devon Ice Cap. We provide estimates of cumulative PFCA deposition globally. We find that given the most recent emission inventory, the atmospheric source of PFCAs is 6-185 tonnes per year globally and 0.1-2.1 tonnes per year to the Arctic.
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PFASs are carried through the atmosphere in both gas and particle forms, enabling their transport over long distances from their initial sources.
“PFASs are carried through the atmosphere in both gas and particle forms, enabling their transport over long distances from their initial sources [96,97].”
From Industrial Applications, Environmental Fate, Human Exposure, and Health Effects of PFAS (2025) · cites this paper as [97]
The Introduction says PFCAs and their precursors have been detected far from emission sources, and the Discussion distinguishes particle-bound PFCAs from gas-phase PFCAs. But the model does not resolve particle partitioning, so the paper does not establish that transport in both forms enables long-distance movement of PFASs generally. The Discussion also says particle association becomes important particularly for long-chain PFCAs. (LLM, conf=0.84)
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References 54 · Cited by 78
Research works printed but not linked: 54
- [1]Wang Z, Cousins IT, Scheringer M, Buck RC and Hungerbuhler K, Environment International, 2014, 70, 62– 75. 24932785
- [2]Martin JW, Mabury SA, Solomon KR and Muir DCG, Environ. Toxicol. Chem, 2003, 22, 189– 195. 12503764
- [3]Martin JW, Mabury SA, Solomon KR and Muir DCG, Environ. Toxicol. Chem, 2003, 22, 196– 204. 12503765
- [4]Conder JM, Hoke RA, de Wolf W, Russell MH and Buck RC, Environ. Sci. Technol, 2008, 42, 995– 1003. 18351063
- [5]Young CJ, Furdui VI, Franklin J, Koerner RM, Muir DCG and Mabury SA, Environ. Sci. Technol, 2007, 41, 3455– 3461. 17547163
- [6]Shoeib M, Harner T and Vlahos P, Environ. Sci. Technol, 2006, 40, 7577– 7583. 17256497
- [7]Stock NL, Furdui VI, Muir DCG and Mabury SA, Environ. Sci. Technol, 2007, 41, 3529– 3536. 17547174
- [8]Xie Z, Wang Z, Mi W, Moller A, Wolschke H and Ebinghaus R, Scientific Reports, 2015, 5, year. PMC4352854 25746440
- [9]Scott BF, Spencer C, Mabury SA and Muir DCG, Environ. Sci. Technol, 2006, 40, 7167– 7174. 17180963
- [10]Houde M, Martin JW, Letcher RJ, Solomon KR and Muir DCG, Environ. Sci. Technol, 2006, 40, 3463– 3473. 16786681
- [11]Ellis DA, Martin JW, Mabury SA, Hurley MD, Andersen MPS and Wallington TJ, Environ. Sci. Technol, 2003, 37, 3816– 3820. 12967100
- [12]Young CJ and Mabury SA, Reviews of environmental contamination and toxicology, 2010, 208, 1– 109. 20811862
- [13]Waterland RL and Dobbs KD, J. Phys. Chem. A, 2007, 111, 2555– 2562. 17388359
- [14]Chiappero MS, Malanca FE, Arguello GA, Wooldridge ST, Hurley MD, Ball JC, Wallington TJ, Waterland RL and Buck RC, J. Phys. Chem. A, 2006, 110, 11944– 11953. 17064182
- [15]Yarwood G, Kemball-Cook S, Keinath M, Waterland RL, Korzeniowski SH, Buck RC, Russell MH and Washburn ST, Environ. Sci. Technol, 2007, 41, 5756– 5762. 17874783
- [16]Thackray CP and Selin NE, Atmos. Chem. Phys, 2017, 17, 4585– 4597.
- [17]Vierke L, Staude C, Biegel-Engler A, Drost W and Schulte C, Environmental Sciences Europe, 2012, 24, 1– 11. PMC5834591 29527446
- [18]Wallington TJ, Hurley MD, Xia J, Wuebbles DJ, Sillman S, Ito A, Penner JE, Ellis DA, Martin J, Mabury SA, Nielsen OJ and Andersen MPS, Environ. Sci. Technol, 2006, 40, 924– 930. 16509338
- [19]Wang Z, Cousins IT, Scheringer M, Buck RC and Hungerbuhler K, Environment International, 2014, 69, 166– 176. 24861268
- [20]Young CJ, Hurley MD, Wallington TJ and Mabury SA, J. Phys. Chem. A, 2008, 112, 13542– 13548. 19053571
- [21]Butt CM, Young CJ, Mabury SA, Hurley MD and Wallington TJ, J. Phys. Chem. A, 2009, 113, 3155– 3161. 19275140
- [22]Schenker U, Scheringer M, Macleod M, Martin JW, Cousins IT and Hungerbuhler K, Environ. Sci. Technol, 2008, 42, 3710– 3716. 18546712
- [23]Bey I, Jacob DJ, Yantosca RM, Logan JA, Field B, Fiore AM, Li Q, Liu H, Mickley LJ and Schultz M, J. Geophys. Res, 2001, 106, 23073– 23096.
- [25]Liu H, Jacob DJ, Bey I and Yantosca RM, J. Geosphys. Res, 2001, 106, 12109– 12128.
- [26]Wang Y, Jacob DJ and Logan JA, J. Geophys. Res, 1998, 103, 10713– 10726.
- [27]Prevedouros K, Cousins IT, Buck RC and Korzeniowski SH, Environ. Sci. Technol, 2006, 40, 32– 44. 16433330
- [28]Arp HP, Niederer C and Goss K-U, Environmental Science and Technology, 2006, 40, 7298– 7304. 17180981
- [29]Stemmler I and Lammel G, Atmospheric Chemistry and Physics, 2010, 10, 9965– 9980.
- [30]Johansson J, Salter M, Navarro JA, Leck C, Nilsson E and Cousins I, Environ. Sci.: Processes and Impacts, 2019, 21, 635– 649. 30888351
- [31]Pickard HM, Criscitiello AS, Spencer C, Sharp MJ, Muir DCG, Silva AOD and Young CJ, Atmospheric Chemistry and Physics, 2018, 18, 5045– 5058.
- [32]Kwok K, Taniyasu S, Yeung L, Murphy M, Lam P, Horii Y, Kannan K, Petrick G, Sinha R and Yamashita N, Environ. Sci. Technol, 2010, 44, 7043– 7049. 20795671
- [33]Kirchgeorg T, Dreyer A, Gabrieli J, Kehrwald N, Sigl M, Schwikowski M, Boutron C, Gambaro A, Barbante C and Ebinghaus R, Environ. Pollut, 2013, 178, 367– 374. 23607941
- [34]Barton C, Kaiser M and Russell M, J. Environ. Monitor, 2007, 9, 839– 846. 17671665
- [35]Kim S-K and Kannan K, Environ. Sci. Technol, 2007, 41, 8328– 8334. 18200859
- [36]Loos R, Wollgast J, Huber T and Hanke G, Anal. Bioanal. Chem, 2007, 387, 1469– 1478. 17200857
- [37]Taniyasu S, Kannan K, Yeung L, Kwok K, Lam P and Yamashita N, Anal. Chem. Acta, 2008, 619, 221– 230. 18558116
- [38]Liu W, Dong G, Jin Y, Sasaki K, Saito N, Sato I, Tsuda S and Nakayama S, Chin. Sci. Bull, 2009, 54, 2440– 2445.
- [39]Liu W, Jin Y, Quan X, Sasaki K, Saito N, Nakayama S, Sato I and Tsuda S, Environ. International, 2009, 35, 737– 742. 19278728
- [40]Mahmoud M, Karrman A, Oono S, Harada K and Koizumi A, Chemosphere, 2009, 74, 467– 472. 19081600
- [41]Murakami M, Shinohara H and Takada H, Chemosphere, 2009, 74, 487– 493. 19054542
- [42]Dreyer A, Matthias V, Weinberg I and Ebinghaus R, Environ. Pollut, 2010, 158, 1221– 1227. 20185217
- [43]Scott B, Silva AD, Spencer C, Lopez E, Backus S and Muir D, J. Great Lakes Res, 2010, 36, 277– 284.
- [44]Zhang X, Niu H, Pan Y, Shi Y and Cai Y, Anal. Chem, 2010, 82, 2363– 2371. 20155948
- [45]Meyer T, Silva AD, Spencer C and Wania F, Environ. Sci. Technol, 2011, 45, 8113– 8119. 21692458
- [46]Muller C, Spiess N, Gerecke A, Scheringer M and Hungerbuhler K, Environ. Sci. Technol, 2011, 45, 9901– 9909. 22035097
- [47]Nguyen V, Reinhard M and Karina G-H, Chemosphere, 2011, 82, 1277– 1285. 21208640
- [48]Nishikoori H, Murakami M, Sakai H, Oguma K, Takada H and Takizawa S, Chemosphere, 2011, 84, 1125– 1132. 21546052
- [49]Zhao X, Cai Y, Wu F, Pan Y, Liao H and Xu B, Microchem. J, 2011, 2011, 98.
- [50]Thackray CP, Friedman CL, Zhang Y and Selin NE, Environ. Sci. Technol, 2015, 49, 9185– 9193. 26110215 PMC4786340
- [51]Chen Y-H and Prinn RG, Journal of Geosphysical Research, 2006, 111, D10307.
- [52]Li L, Liu J, Hu J and Wania F, Environ. Sci. Technol, 2017, 51, 4461– 4470. 28301932
- [53]Washington J, Rankin K, Libelo E, Lynch D, and Cyterski M, Sci. Total Environ, 2019, 651, 2444– 2449. 30336434 PMC7957346
- [54]Wania F, Environ. Sci. Technol, 2007, 41, 4529– 4535. 17695892
- [55]Ahrens L, Harner T, Shoeib M, Lane DA and Murphy JG, Environmental Science and Technology, 2012, 46, 7199– 7206. 22606993
- Authors
- Thackray, C. P., Selin, N. E., & Young, C. J.
- Affiliations
- Massachusetts Institute of Technology (US)
- York University (CA)
- Corresponding author
- Thackray, Colin P.
- Venue
- Environmental Science: Processes & Impacts
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2020
- Volume
- 22
- Issue
- 2
- Pages
- 285-293
- ISSN
- 2050-7887 (ISSN-L)
- 2050-7895
- PMC
- PMC7050637
- OpenAlex
- W2998285627
- Cited by
- 78
- References
- 54
- Citations by year
- 2026: 14 · 2025: 16 · 2024: 14 · 2023: 11 · 2022: 8 · 2021: 9 · 2020: 5 · 2019: 1
- FWCI
- 2.50
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Locations
- Environmental Science Processes & Impacts (publishedVersion, cc-by)
- PubMed (publishedVersion)
- Europe PMC (PubMed Central) (acceptedVersion)
- PubMed Central (acceptedVersion)
- DSpace@MIT (Massachusetts Institute of Technology) (submittedVersion, cc-by-nc)
- Funders
- National Science Foundation (1203526)
- National Institute of Environmental Health Sciences (3P42ES027707-03S1)
- Natural Sciences and Engineering Research Council of Canada
- Topics
- Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
- Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
- Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric Ozone and Climate
- Keywords
- perfluorocarboxylic acids, fluorotelomer alcohols, atmospheric transport, atmospheric deposition, GEOS-Chem
- MeSH terms
- Air Movements, Arctic Regions, Carboxylic Acids, Fluorocarbons, Models, Chemical
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