Catalytic reactive-hydrogen membranes for rapid capture and hydrodefluorination of six PFAS of regulatory concern
6 affiliations
- 1State Key Laboratory of Water Pollution Control and Green Resource Recycling, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
- 2Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, AZ 85287-5701
- 3Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005-1892
- 4Institute for the Environment and Health, Nanjing University, Suzhou 215163, China
- 5State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
- 6Department of Chemical and Biomolecular Engineering, Institute for Functional Intelligent Materials, National University of Singapore, Singapore 119077, Singapore
Abstract
Per- and polyfluoroalkyl substances (PFAS) persist in aquatic environments due to their ultrastable C–F bonds and poor susceptibility to conventional treatment. Here, we report an H2-based catalytic-film membrane that enables PFAS destruction in ambient conditions by generating highly reactive surface (Hads*) and subsurface hydrogen (Hsub*), the latter stored as β-phase palladium hydride (β-PdHx). Solid-state analyses evidenced β-PdHx formation and related lattice expansion with elevated H2 chemical potential, revealing a structural mechanism that links hydrogen storage to catalytic defluorination. Mechanistically, the two hydrogen species play complementary roles: Hads*-rich Pd0 surface enabled PFAS capture through parallel adsorption to maximize interfacial contact with active H, whereas sustained Hsub* supplied the energetic driving force for stepwise hydrodefluorination consistent with sequential C–F scission. As a result, across six PFAS of regulatory concern—PFOA, PFOS, PFNA, PFHxS, PFBS, and GenX—the catalytic membrane converted all contaminants toward fully defluorinated products. Long-chain PFAS were removed and defluorinated more rapidly than short-chain analogs, while GenX showed greater recalcitrance due to its ether linkage, weaker adsorption, and higher average C–F bond dissociation energy; nonetheless, GenX still exhibited removal and defluorination, with the production of 2-propoxypropanoic acid. The system also enabled continuous coremoval of all six PFAS in ambient conditions, with up to 96% removal and 83% defluorination over 58 d. These findings provide a mechanistic framework for how active hydrogen is generated, stored, and deployed in catalytic membranes, and identify engineered H2-catalytic membranes as a promising low-energy technology for destructive PFAS treatment.
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BibTeX
@article{long2026catalytic,
title = {{Catalytic reactive-hydrogen membranes for rapid capture and hydrodefluorination of six PFAS of regulatory concern}},
author = {Min Long and Ai-Shi Wang and Welman C. Elias and Chen Zhou and Thomas P. Senftle and Michael S. Wong and Jie Cheng and Bruce E. Rittmann},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
year = {2026},
month = oct,
doi = {10.1073/pnas.2613985123},
url = {https://doi.org/10.1073/pnas.2613985123},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Catalytic reactive-hydrogen membranes for rapid capture and hydrodefluorination of six PFAS of regulatory concern
AU - Min Long
AU - Ai-Shi Wang
AU - Welman C. Elias
AU - Chen Zhou
AU - Thomas P. Senftle
AU - Michael S. Wong
AU - Jie Cheng
AU - Bruce E. Rittmann
PY - 2026
DA - 2026/10/19
JO - Proceedings of the National Academy of Sciences of the United States of America
DO - 10.1073/pnas.2613985123
UR - https://doi.org/10.1073/pnas.2613985123
AB - Per- and polyfluoroalkyl substances (PFAS) persist in aquatic environments due to their ultrastable C–F bonds and poor susceptibility to conventional treatment. Here, we report an H2-based catalytic-film membrane that enables PFAS destruction in ambient conditions by generating highly reactive surface (Hads*) and subsurface hydrogen (Hsub*), the latter stored as β-phase palladium hydride (β-PdHx). Solid-state analyses evidenced β-PdHx formation and related lattice expansion with elevated H2 chemical potential, revealing a structural mechanism that links hydrogen storage to catalytic defluorination. Mechanistically, the two hydrogen species play complementary roles: Hads*-rich Pd0 surface enabled PFAS capture through parallel adsorption to maximize interfacial contact with active H, whereas sustained Hsub* supplied the energetic driving force for stepwise hydrodefluorination consistent with sequential C–F scission. As a result, across six PFAS of regulatory concern—PFOA, PFOS, PFNA, PFHxS, PFBS, and GenX—the catalytic membrane converted all contaminants toward fully defluorinated products. Long-chain PFAS were removed and defluorinated more rapidly than short-chain analogs, while GenX showed greater recalcitrance due to its ether linkage, weaker adsorption, and higher average C–F bond dissociation energy; nonetheless, GenX still exhibited removal and defluorination, with the production of 2-propoxypropanoic acid. The system also enabled continuous coremoval of all six PFAS in ambient conditions, with up to 96% removal and 83% defluorination over 58 d. These findings provide a mechanistic framework for how active hydrogen is generated, stored, and deployed in catalytic membranes, and identify engineered H2-catalytic membranes as a promising low-energy technology for destructive PFAS treatment.
SN - 0027-8424
SN - 1091-6490
ER -