Catalytic reactive-hydrogen membranes for rapid capture and hydrodefluorination of six PFAS of regulatory concern.

Authors

Min Long, Ai-Shi Wang, Welman C Elias, Chen Zhou, Thomas P Senftle, Michael S Wong, Jie Cheng, Bruce E Rittmann

Published in

Proceedings of the National Academy of Sciences of the United States of America. Volume 123. Issue 43. Pages e2613985123. Oct 27, 2026. Epub Oct 19, 2026.

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 (H_ads^*) and subsurface hydrogen (H_sub^*), 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: H_ads^*-rich Pd⁰ surface enabled PFAS capture through parallel adsorption to maximize interfacial contact with active H, whereas sustained H_sub^* 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.

PMID:
42896056
Bibliographic data and abstract were imported from PubMed on 20 Oct 2026.

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