Title: Investigating the Atmospheric Sources and Sinks of Perfluorooctanoic Acid Using a Global Chemistry Transport Model

Abstract

Perfluorooctanoic acid, PFOA, is one of the many concerning pollutants in our atmosphere; it is highly resistant to environmental degradation processes, which enables it to accumulate biologically. With direct routes of this chemical to the environment decreasing, as a consequence of the industrial phase out of PFOA, it has become more important to accurately model the effects of indirect production routes, such as environmental degradation of precursors; e.g., fluorotelomer alcohols (FTOHs). The study reported here investigates the chemistry, physical loss and transport of PFOA and its precursors, FTOHs, throughout the troposphere using a 3D global chemical transport model, STOCHEM-CRI. Furthermore, this investigation includes an important loss process of PFOA in the atmosphere via the addition of the stabilised Criegee intermediates, hereby referred to as the “Criegee Field.” Whilst reaction with Criegee intermediates is a significant atmospheric loss process of PFOA, it does not result in its permanent removal from the atmosphere. Additionally, the atmospheric fate of the resultant hydroperoxide product from the reaction of PFOA and Criegee intermediates resulted in a ≈0.04 Gg year-1 increase in the production flux of PFOA. Furthermore, the physical loss of the hydroperoxide product from the atmosphere (i.e., deposition), whilst decreasing the atmospheric concentration, ismore » also likely to result in the reformation of PFOA in environmental aqueous phases, such as clouds, precipitation, oceans and lakes. As such, removal facilitated by the “Criegee Field” is likely to simply result in the acceleration of PFOA transfer to the surface (with an expected decrease in PFOA atmospheric lifetime of ≈10 h, on average from ca. 80 h without Criegee loss to 70 h with Criegee loss).« less

Authors:

Holland, Rayne  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-1975-0587"

Khan, M. Anwar H.  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-7836-3344"

Chhantyal-Pun, Rabi  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-7515-0108"

Orr-Ewing, Andrew J.  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-5551-9609"

Percival, Carl J. ^[2]; Taatjes, Craig A.  ^[3];

• Search DOE PAGES for author "Taatjes, Craig A."
• Search DOE PAGES for ORCID "0000-0002-9271-0282"

Shallcross, Dudley E. ^[4]

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+ Show Author Affiliations

1. Univ. of Bristol (United Kingdom)
2. California Institute of Technology (CalTech), Pasadena, CA (United States). Jet Propulsion Lab. (JPL)
3. Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
4. Univ. of Bristol (United Kingdom); Univ. of the Western Cape, Bellville (South Africa)

Publication Date:

Sun Apr 19 00:00:00 EDT 2020

Research Org.:

Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); NERC; USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:

1644076

Report Number(s):

SAND-2020-7176J
Journal ID: ISSN 2073-4433; 687347

Grant/Contract Number:  

AC04-94AL85000; NE/K004905/1; NE/I014381/1; NE/P013104/1; AC02-05CH11231; NA0003525

Resource Type:

Accepted Manuscript

Journal Name:

Atmosphere (Basel)

Additional Journal Information:

Journal Name: Atmosphere (Basel); Journal Volume: 11; Journal Issue: 4; Journal ID: ISSN 2073-4433

Publisher:

MDPI

Country of Publication:

United States

Language:

English

Subject:

54 ENVIRONMENTAL SCIENCES; Criegee intermediates; perfluorooctanoic acid; global budget; atmospheric lifetime