Cited by 78Per- and polyfluoroalkyl substances researchAtmospheric chemistry and aerosolsAtmospheric Ozone and Climate

A global atmospheric chemistry model for the fate and transport of PFCAs and their precursors

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Thackray, Colin P., Selin, Noelle E., Young, Cora J.·2020·Environmental Science: Processes & Impacts

Abstract

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

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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
Published
2020
Volume
22
Issue
2
Pages
285-293
ISSN
  • 2050-7887 (ISSN-L)
  • 2050-7895
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
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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