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Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation
https://orcid.org/0000-0003-2508-0644
https://orcid.org/0000-0003-0907-5626
https://orcid.org/0000-0002-1441-0401
https://orcid.org/0000-0001-9635-5807
https://orcid.org/0000-0002-1575-5946
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.
Co-NPs fine-tune the electronic structure of Co-SA sites, optimizing PMS adsorption and activation to generate confined reactive species.
Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation
https://orcid.org/0000-0003-2508-0644
https://orcid.org/0000-0003-0907-5626
https://orcid.org/0000-0002-1441-0401
https://orcid.org/0000-0001-9635-5807
https://orcid.org/0000-0002-1575-5946
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.
Co-NPs fine-tune the electronic structure of Co-SA sites, optimizing PMS adsorption and activation to generate confined reactive species.
Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation
https://orcid.org/0000-0003-2508-0644
https://orcid.org/0000-0003-0907-5626
https://orcid.org/0000-0002-1441-0401
https://orcid.org/0000-0001-9635-5807
https://orcid.org/0000-0002-1575-5946
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.
Co-NPs fine-tune the electronic structure of Co-SA sites, optimizing PMS adsorption and activation to generate confined reactive species.
Single-Atom Cobalt Catalysts Encapsulating Cobalt Nanoparticles with Built-In Electric Field for Ultrafast and Lasting Peroxymonosulfate Activation
Zou, Haiyan (author) / Wang, Haitao (author) / Sun, Hongqi (author) / Sun, Wenshuang (author) / Luo, Shuangjiang (author) / Li, Tielong (author) / Duan, Xiaoguang (author) / Zhan, Sihui (author)
ACS ES&T Water ; 4 ; 2433-2444
2024-06-14
Article (Journal)
Electronic Resource
English
| American Chemical Society | 2024
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