A global atmospheric chemistry model for the fate and transport of PFCAs and their precursors
Name
c9em00326f.pdf
Description
Published version
Size
661.37 KB
Format
Adobe PDF
Checksum (MD5)
56c67b561b00210f362500e2a7aca38c
Author(s)
Thackray, Colin P
Selin, Noelle E
Young, Cora J
Date Issued
2020
Journal
Environmental Science: Processes & Impacts
Publisher
Royal Society of Chemistry (RSC)
Version
Final published version
Abstract
© 2020 The Royal Society of Chemistry. 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.
MIT Department
Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences
Terms of Use
Creative Commons Attribution 4.0 International license
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1039/C9EM00326F
