Issue 2, 2023

Exploring controls on perfluorocarboxylic acid (PFCA) gas–particle partitioning using a model with observational constraints

Abstract

The atmospheric fate of perfluorocarboxylic acids (PFCAs) has attracted much attention in recent decades due to the role of the atmosphere in global transport of these persistent chemicals. There is a gap in our understanding of gas–particle partitioning, limited by availability of reliable atmospheric measurements, partitioning properties, and models of gas–particle interactions. The gas–particle equilibrium phase partitioning of C2–C16 PFCAs in the atmosphere were modeled here by taking account of both deprotonation and phase partitioning equilibria among air, aerosol liquid water, and particulate water-insoluble organic matter using a range of available PFCA partitioning properties. We systematically varied water and organic matter content to simulate the full range of atmospheric conditions. Except in severe organic matter pollution episodes, shorter-chain PFCAs are predicted to mainly partition between air and aqueous phase, while for PFCAs with carbon chains longer than 12, organic matter is more likely to be the dominant particle phase reservoir. The model framework underestimated the particle fraction of C2–C8 PFCAs compared with several ambient observations, with larger discrepancies observed for longer-chain PFCAs. The discrepancy could result from externally mixed dust components, non-ideality of aerosol liquid water, surfactant descriptions at phase boundaries, and missed interactions between organic matter and charged PFCA molecules. Reliable measurements of ambient PFCAs with high time resolution and the measurement of uptake parameters by particle-relevant components will be beneficial to more reliable environmental fate modeling of ambient PFCAs.

Graphical abstract: Exploring controls on perfluorocarboxylic acid (PFCA) gas–particle partitioning using a model with observational constraints

Supplementary files

Article information

Article type
Paper
Submitted
15 Juu 2022
Accepted
03 Seb 2022
First published
05 Seb 2022

Environ. Sci.: Processes Impacts, 2023,25, 264-276

Exploring controls on perfluorocarboxylic acid (PFCA) gas–particle partitioning using a model with observational constraints

Y. Tao, T. C. VandenBoer, R. Ye and C. J. Young, Environ. Sci.: Processes Impacts, 2023, 25, 264 DOI: 10.1039/D2EM00261B

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements