数字农科院2.0

Fe[sbnd]O[sbnd]Co bimetallic bridge-mediated oxygen vacancy formation: Mechanism of synergistic activation of PMS degradation of atrazine

文献类型： 外文期刊

作者： Bingyang Liu;Yu Wang;Qi Yang;Xiaojing Li

作者机构：

关键词： Atrazine;FeCo-MIL-101;Oxygen vacancy;Peroxymonosulfate

期刊名称： Separation and Purification Technology

ISSN： 1873-3794

年卷期： 2025 年 380 卷

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： Atrazine (ATZ), a highly persistent triazine herbicide, poses significant environmental risks due to its endocrine-disrupting effects, necessitating efficient remediation technologies. To overcome the limitations of active site availability and electron transfer bottlenecks in single-metal iron-based MOFs (Fe-MIL-101) during peroxymonosulfate (PMS) activation, this study innovatively constructed bimetallic FeM-MIL-101 (M = Co, Zn, Ni, Cu) catalysts. Through hydrothermal synthesis and multi-scale characterization, FeCo-MIL-101 was shown to achieve complete ATZ degradation within 60 min (kobs = 0.059 min−1), representing a 3.9-fold enhancement in degradation efficiency over the best-performing control. The catalyst maintained >95 % removal efficiency across a broad pH range and under interference from high concentrations of common anions (Cl−, NO3−, SO42−, H2PO4−), while exhibiting minimal inhibition by HCO3− (>82 % removal). Mechanistic studies revealed that Fe[sbnd]O[sbnd]Co bridging bonds induced oxygen vacancy (OV) generation, significantly accelerating the Fe3+/Co3+ ↔ Fe2+/Co2+ redox cycles and synergistically optimizing both radical and non-radical pathways. Sulfate radicals (SO4[rad]–) served as the dominant reactive species (contributing 58.3 %), with singlet oxygen (1O2) and superoxide radicals (O2[rad]–) playing a synergistic role (collectively 38 %). The catalyst retained >90 % activity over 6 consecutive cycles, with metal leaching below 14 μg/L, and the degradation products exhibited significantly reduced developmental toxicity. Bimetallic synergy and OV-mediated electron transfer were identified as the key factors enhancing PMS activation efficiency. By strengthening HSO5− adsorption energy and interfacial charge transfer, FeCo-MIL-101 overcomes the limitations of single-metal systems, providing an atomic-level design strategy for the efficient removal of persistent organic pollutants in complex aqueous environments.

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