成果归属作者：

杨琦

成果归属机构：

水资源与环境学院

作者：

Liu, Bingyang ; Wang, Yu ; Yang, Qi ; Li, Xiaojing

单位：

Minist Agr & Rural Affairs, Agroenvironm Protect Inst, MARA, Key Lab Original Agroenvironm Pollut Prevent & Con, Tianjin Key Lab Agroenvironm & Agroprod Safety, Tianjin 300191, Peoples R China;China Univ Geosci Beijing, Beijing Key Lab Water Resources & Environm Engn, Beijing 100083, Peoples R China;Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Cont, Beijing 100084, Peoples R China

关键词：

GRAPHENE

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 (k(obs) = 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 FeOCo 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-) served as the dominant reactive species (contributing 58.3 %), with singlet oxygen (O-1(2)) and superoxide radicals (O-2(-)) playing a synergistic role (collectively 38 %). The catalyst retained >90 % activity over 6 consecutive cycles, with metal leaching below 14 mu g/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.

基金：

Agricultural Science and Technology Innovation Program [CAAS-CSGLCA-202502]; National Natural Science Foundation of China [42477041, 41977133]; Natural Science Foundation of Tianjin [23JCZDJC00480]

语种：

英文

DOI：

10.1016/j.seppur.2025.135345

来源：

SEPARATION AND PURIFICATION TECHNOLOGY,2026():.

出版日期：

2026-02-07

提交日期：

2025-11-15

引用参考：

Liu, Bingyang; Wang, Yu; Yang, Qi; Li, Xiaojing. Fe-O-Co bimetallic bridge-mediated oxygen vacancy formation: Mechanism of synergistic activation of PMS degradation of atrazine[J]. SEPARATION AND PURIFICATION TECHNOLOGY,2026():.