Cobalt Single Atoms Anchored on Oxygen-Doped Tubular Carbon Nitride for Efficient Peroxymonosulfate Activation: Simultaneous Coordination Structure and Morphology Modulation.
Cobalt Single Atoms Anchored on Oxygen-Doped Tubular Carbon Nitride for Efficient Peroxymonosulfate Activation: Simultaneous Coordination Structure and Morphology Modulation.
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DOI：
10.1002/anie.202202338
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发表时间：
2022-05
影响因子：
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通讯作者：
Ziwei Wang;Eydhah Almatrafi;Han Wang;Hong Qin;Wenjun Wang;Li Du;Shan Chen;G. Zeng;Piao Xu
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文献类型：
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作者：
Ziwei Wang;Eydhah Almatrafi;Han Wang;Hong Qin;Wenjun Wang;Li Du;Shan Chen;G. Zeng;Piao Xu
同时调节单原子催化剂的配位环境和具有有效暴露活性位点的工程结构是促进过一硫酸盐（PMS）活化的有效策略。通过热解氰尿酸-三聚氰胺-醋酸钴的氢键前驱体，在掺氧管状氮化碳（TCN）上分离出具有氮氧双配位的钴原子（Co-N3 O 1）。理论上构建的Co-N3 O 1结构单元具有7.61×105 min-1 mol-1的质量活度和较高的1 O2选择性.理论计算表明，钴单原子占据了氮氧双配位环境，促进了PMS吸附，降低了生成1 O2的关键 *O中间体的能垒.将催化剂连接到广泛使用的聚（偏二氟乙烯）微滤膜上，以在10小时内提供具有97.5%环丙沙星截留率的抗生素废水处理系统，从而揭示了膜用于工业应用的适用性。
Simultaneous regulation of the coordination environment of single-atom catalysts and engineering architectures with efficient exposed active sites are efficient strategies for boosting peroxymonosulfate (PMS) activation. We isolated cobalt atoms with dual nitrogen and oxygen coordination (Co-N 3 O 1 ) on oxygen-doped tubular carbon nitride (TCN) by pyrolyzing a hydrogen-bonded cyanuric acid melamine-cobalt acetate precursor. The theoretically constructed Co-N 3 O 1 moiety on TCN exhibited an impressive mass activity of 7.61×105 min -1 mol -1 with high 1 O 2 selectivity. Theoretical calculations revealed that the cobalt single atoms occupied a dual nitrogen and oxygen coordination environment, and that PMS adsorption was promoted and energy barriers reduced for the key *O intermediate that produced 1 O 2 . The catalysts were attached to a widely used poly(vinylidene fluoride) microfiltration membrane to deliver an antibiotic wastewater treatment system with 97.5% ciprofloxacin rejection over 10 hours, thereby revealing the suitability of the membrane for industrial applications.