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Synergy of Fe-Nx Sites and Oxygen Vacancies Enables Radical and Nonradical Pathways in Peroxymonosulfate Activation

文献类型： 外文期刊

作者： 李雪;李良玉;王军捷;郭海心;孙约兵;张祖麟;杨凤霞;丁永祯

关键词： Fe–Nx; sites Oxygen vacancy; Peroxymonosulfate activation; Interfacial electron transfer; Reactive oxygen species

期刊名称： Chemical Engineering Journal

ISSN： 1385-8947

年卷期： 2025 年

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： Fe–N–C catalysts are promising peroxymonosulfate (PMS) activators, yet their tendency for Fe–Nx site ag gregation and rigid electronic environments restricts the concurrent activation of radical and nonradical path ways. Here, we developed a one-step ball-milling strategy that yields a dual-site catalyst (Fe–N@C-500-3) enriched with oxygen vacancies, stabilizing Fe–Nx sites and modulating the electronic environment. Fe–N@C- 500-3 reached a reaction rate constant of 0.10 min 1 for sulfamethoxazole (SMX) degradation, which is one order of magnitude higher than pristine Fe–N@C and superior to most reported Fe–N–C catalysts. Fe–N@C- 500-3 delivered excellent degradation activity toward diverse micropollutants and showed strong resistance to environmental interferences. It further sustained efficiency in continuous-flow operation, maintained stability through multiple cycles, and achieved 85.5 % SMX removal from real livestock wastewater. Mechanistic analysis revealed that PMS activation initiated through inner-sphere coordination at Fe–Nx sites to form PMS-derived intermediates (PMS*). Ov induced charge delocalization and optimized the d-band electronic structure of adjacent Fe centers. The synergy of Fe–Nx sites and Ov lowered the barrier for PMS* formation, thereby pro moting interfacial electron transfer and enhancing reactive oxygen species generation. This work elucidates the mechanistic role of Fe–Nx/Ov synergy in PMS activation and provides a scalable strategy for advanced water treatment.

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