Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation

催化作用 纳米颗粒 电子转移 吸附 化学 金属 材料科学 化学工程 光化学 纳米技术 无机化学 物理化学 有机化学 工程类
作者
Haiyan Zou,Haitao Wang,Hongqi Sun,Wenshuang Sun,Shuangjiang Luo,Tielong Li,Xiaoguang Duan,Sihui Zhan
出处
期刊:ACS ES&T water [American Chemical Society]
卷期号:4 (6): 2433-2444 被引量:1
标识
DOI:10.1021/acsestwater.3c00774
摘要

Cobalt single-atom catalysts (Co-SAs) are rising stars in persulfate chemistry for their well-defined coordination, reduced metal usage, and exceptional activity. However, the simultaneous formation of cobalt nanoparticles (Co-NPs) with Co-SAs raises questions about their complex interplay and synergy in catalysis. In this study, we synthesized Co-SAs-encapsulated Co-NPs (CoNP@NC/Co-SA) using the laser-induced carbonization strategy of high entropy synthesis technology. The results show that 93.23% of phenol can be removed in 15 min and 91.60% in 3 min in the CoNP@NC/Co-SA/PMS system. Simulation results showed that Co-NPs fine-tune the electronic structure of Co-SA sites, optimizing PMS adsorption and activation to generate confined reactive species. The surface-activated PMS-catalyst complex directly attacked adsorbed pollutants on the catalyst surface via an electron-transfer regime. CoNP@NC/Co-SA catalyzes PMS oxidation through a nonradical pathway with high selectivity toward target organics. The findings emphasize the synergistic effect of Co-SAs and Co-NPs in promoting Fenton-like catalysis, enlightening the rational design of advanced composite materials via synergistic molecular and interfacial engineering for fast and long-lasting catalytic oxidation. At the same time, this work provides insights into the electronic structure regulation of metal centers at the atomic level.
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