Acidity-Driven Spontaneous Degradation of Trifluoroacetic Acid at Droplet Air–Water Interfaces
Abstract
Trifluoroacetic acid (TFA), an ultrashort-chain per- and polyfluoroalkyl substance, is increasingly detected in the environment and has raised widespread concern because of its negative effects on health and ecosystems. However, whether TFA can degrade naturally in the environment remains unresolved. Here, we report the spontaneous degradation of TFA at the air–water interface of droplets, yielding F– and fluorine-containing transformation products, including CHF3O, CF3O2H, and CH2F2O2. The extent of degradation is strongly dependent on droplet acidity, with the F– yield at pH 10 being 12-fold higher than at pH 5. Density functional theory calculations reveal a mechanism favored by alkaline conditions and oxygen in which interfacial decarboxylation triggers sequential oxidation and defluorination. These findings identify the air–water interface of pH-regulated droplets as a reactive microenvironment for spontaneous TFA degradation, offering new insights into the environmental transformation of ultrashort-chain PFAS.
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BibTeX
@article{chen2026aciditydriven,
title = {{Acidity-Driven Spontaneous Degradation of Trifluoroacetic Acid at Droplet Air–Water Interfaces}},
author = {Y. Chen and J. Lin and Z. Sun and H. Xiong and Z. Guo and X. Wang and R. Zhang and S. Liu and W. Wu and Q. X. Li and L. Zhang and A. Mellouki and C. George and J. Chen},
journal = {Journal of the American Chemical Society},
year = {2026},
month = nov,
doi = {10.1021/jacs.6c14844},
url = {https://hal.science/hal-05851345v1},
note = {CC BY-NC-ND},
}
RIS
TY - JOUR
TI - Acidity-Driven Spontaneous Degradation of Trifluoroacetic Acid at Droplet Air–Water Interfaces
AU - Y. Chen
AU - J. Lin
AU - Z. Sun
AU - H. Xiong
AU - Z. Guo
AU - X. Wang
AU - R. Zhang
AU - S. Liu
AU - W. Wu
AU - Q. X. Li
AU - L. Zhang
AU - A. Mellouki
AU - C. George
AU - J. Chen
PY - 2026
DA - 2026/11/04
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c14844
UR - https://hal.science/hal-05851345v1
AB - Trifluoroacetic acid (TFA), an ultrashort-chain per- and polyfluoroalkyl substance, is increasingly detected in the environment and has raised widespread concern because of its negative effects on health and ecosystems. However, whether TFA can degrade naturally in the environment remains unresolved. Here, we report the spontaneous degradation of TFA at the air–water interface of droplets, yielding F– and fluorine-containing transformation products, including CHF3O, CF3O2H, and CH2F2O2. The extent of degradation is strongly dependent on droplet acidity, with the F– yield at pH 10 being 12-fold higher than at pH 5. Density functional theory calculations reveal a mechanism favored by alkaline conditions and oxygen in which interfacial decarboxylation triggers sequential oxidation and defluorination. These findings identify the air–water interface of pH-regulated droplets as a reactive microenvironment for spontaneous TFA degradation, offering new insights into the environmental transformation of ultrashort-chain PFAS.
SN - 0002-7863
SN - 1520-5126
ER -