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MOF-derived Fe based catalysts for efficiently Advanced Oxidation Processes: From single atoms to diatomic and nanoparticles

引用

Progress in Natural Science:Materials International 2023年第4期33卷 534-543页

作者： Xinyi Yang Jiewen Qin Zhichao Dai Yunqiang Sun Hongmei Liu Xiuwen Zheng Zunfu Hu School of Chemistry and Chemical Engineering Linyi University Key Laboratory of Advanced Biomaterials and Nanomedicine in Universities of Shandong School of Physics and Electronic Engineering Linyi University Qilu Normal University

Sub-nanometer catalysts have drawn great attention based on their superior catalytic activity and extensive application in advanced oxidation processes(AOPs). Nonetheless, the precise regulation of the coordination environment and exploration of the peroxymonosulfate(PMS) activation mechanism remain the focus of research.Herein, we report the preparation of Fe catalysts with diverse sizes, including single atoms(SAs), double atoms(DAs), and nanoparticles(NPs) via adjusting the precursor. Sub-nanometric Fe catalysts exhibit a higher catalytic activity for Bisphenol A(BPA) degradation. It is confirmed that the catalytic activity of the Fe diatomic catalysts(Fe2–N/C) is 2.5 times that of the Fe single-atom catalysts(Fe1–N/C) and 8.3 times that of the Fe-nanoparticleloaded catalysts(FeNP–N/C). Broad pH adaptation ranges and reusability have also been proved. Based on experimental verification and density functional theory, non-free radical pathways dominate the degradation process of BPA, while free radical pathways are in an auxiliary position, accompanied by electron transfer process.It is found that the synergistic effect of Fe2–N6sites and pyridinic N adsorption centers contribute to the ultra-high catalytic activity of Fe2–N/C. This work opens up an efficient way for single atom catalysts-based advanced oxidation processes for the efficient removal of refractory organic pollutants.

关键词： Advanced oxidation processes double reaction sites Fe diatomic catalysts High efficiency degradation Non-free radical pathways

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