全氟辛酸
脱羧
降级(电信)
化学
基础(拓扑)
路易斯酸
光催化
光化学
环境化学
有机化学
催化作用
计算机科学
电信
数学分析
数学
作者
Wenhui Ding,Tianhao Tang,Xianjun Tan,Yuxiong Huang
标识
DOI:10.1021/acs.est.5c06300
摘要
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.
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