文献类型：期刊文献

英文题名：Harnessing Fe-Mo Atomic Interfaces for Boosted Electron Transfer and ROS Generation in Sustainable Pollutant Degradation

作者：Liang, Lihong[1,2];Cao, Jiazhen[3,4];Chen, Zhuan[1,2];Liang, Zhiyan[1,2];Jiang, Yue[1,2];Xing, Mingyang[1,2,3,4]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Joint Int Res Lab Precis Chem, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Resources & Environm Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Inst Fine Chem, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China

年份：2025

卷号：59

期号：42

起止页码：22914

外文期刊名：ENVIRONMENTAL SCIENCE & TECHNOLOGY

收录：;EI(收录号：20254419409770);WOS:【SCI-EXPANDED(收录号:WOS:001576814400001)】；

基金：This work was supported by the National Natural Science Foundation of China (No. 22325602, 22521201, 22176060) and Program of Shanghai Academic/Technology Research Leader (23XD1421000). Project supported by Shanghai Municipal Science and Technology Major Project (Grant No. 2018SHZDZX03) and the Program of Introducing Talents of Discipline to Universities (B16017). Science and Technology Commission of Shanghai Municipality (20DZ2250400). Authors thank Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：synergistic catalysis; electron transfer; long-termstability; wastewater treatment; single-atom catalysts

摘要：Developing efficient and sustainable catalytic systems for persistent organic pollutant degradation remains a critical challenge in wastewater treatment. Herein, we present a novel FeMo0.5-OCN catalyst integrating iron clusters and molybdenum single atoms with oxygen coordination, which synergistically activates peroxymonosulfate (PMS) to generate reactive oxygen species (ROS), including sulfate radicals (SO4 (center dot-)) and singlet oxygen (O-1(2)), for enhanced pollutant degradation. Density functional theory (DFT) calculations and experimental studies reveal that Mo single atoms facilitate pollutant adsorption via oxygen coordination, while Fe clusters drive PMS activation, enabling efficient electron transfer and ROS generation. The FeMo0.5-OCN/PMS system achieves rapid degradation (>90% within 1 min) and high mineralization (73% TOC removal) of phenol, along with robust stability over 30 reaction cycles and broad pH adaptability (pH 2-11). Apart from phenol, this system demonstrates outstanding degradation efficiency for other phenolic contaminants as well. The practical applicability of the system is demonstrated by chemical oxygen demand (COD) removal efficiencies of 91, 44, and 33% for phenolic, high-salinity, and alcohol-containing wastewaters, respectively, outperforming conventional Fe2+/H2O2 systems and activated carbon treatments. Heterogeneous catalytic model quantifies the contribution of ROS and the mass transfer behaviors of pollutants at the solid-liquid interface. Sensitivity analysis confirms that the O-1(2)-facilitated generation of p-benzoquinone (p-BQ) is the rate-determining step in the overall reaction pathway. Life cycle assessment (LCA) confirms the system's superior environmental sustainability and cost-effectiveness compared to conventional Fenton systems (Fe2+/H2O2 and Fe2+/PMS), with minimal metal leaching. This work highlights the critical role of interfacial electronic interactions in catalytic design and provides a scalable strategy for durable, eco-friendly wastewater remediation.