Enhancing Photocatalytic Decarboxylation by Frustrated Lewis Acid–Base Pairs for Efficient Degradation of Perfluorooctanoic Acid

Recognized as a "forever chemical", perfluorooctanoic acid (PFOA) calls for urgent environmental cleanup. Photocatalytic degradation emerged as a sustainable solution, but it still suffers from sluggish reaction kinetics and insufficient C-F bond cleavage. Addressing the above bottlenecks, we strategically constructed frustrated Lewis acid-base pairs (FLP) on In₂O₃ photocatalyst, which theoretically reduces the PFOA decarboxylation energy by 2.91 eV. The rationally designed In₂O₃-FLP photocatalyst achieved a 23-fold improvement of PFOA degradation rate, a 9-fold increase of defluorination rate, and a 1.6-fold increase of mineralization efficiency compared to pristine In₂O₃. Mechanistic studies reveal that the frustrated Lewis acid (LA) and Lewis base (LB) synergistically facilitate PFOA degradation by enhancing adsorption, promoting charge transfer, and enabling in situ defluorination. This work elucidates mechanistic insights into dual-active-site catalysis via FLP in photocatalytic decarboxylation and proposes a rational photocatalyst design strategy for persistent pollutant remediation.