Surface Density of Cobalt Single Atoms Manipulating Hydroxyl Radical Generation Via Dual Pathways: Electrons Supply and Active sites

Jing Wang; Guangfei Yu; Yuchao WangShenning LiuJiakai QiuYanjun XuZhuan WangYuxian WangYongbing XieHongbin Cao

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Surface Density of Cobalt Single Atoms Manipulating Hydroxyl Radical Generation Via Dual Pathways: Electrons Supply and Active sites

机译：Surface Density of Cobalt Single Atoms Manipulating Hydroxyl Radical Generation Via Dual Pathways: Electrons Supply and Active sites

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Photocatalytic generation of ?OH from O_3 is an intriguing avenue for aqueous organics degradation due to the high utilization of photogenerated electrons, but ambiguous information about charge transfer and surface-active sites hinders the optimization of photocatalysts. In this work, a series of cobalt single-atom catalysts (SACs) anchored on graphitic carbon nitride to improve ?OH generation from O_3 via electron reduction and catalytic activation dual pathway is synthesized. Various characterization and density functional theory calculations reveal that cobalt single atoms can introduce trap states for holes, which improve the light-harvesting ability and accelerate the transfer of electrons and holes. Meanwhile, Co single atoms can also act as active sites to accelerate ozone decomposition and produce ?OH directly. Particularly, the influence of different surface densities of Co single atoms on photogenerated electron supply and surface reaction is disclosed. A higher density of Co provided more active sites for O_3 catalytic activation, but the narrowed distance between oxidation and reduction centers reduces the supply of available electrons by worsening the charge recombination. This work offers an atomic-level correlation of the isolated metal density and photocatalytic properties, and can scientifically guide the design of high-performance photocatalysts for organic synthesis and water purification.

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《Advanced functional materials》 |2023年第21期|2215245.1-2215245.10|共10页
作者
Jing Wang; Guangfei Yu; Yuchao WangShenning LiuJiakai QiuYanjun XuZhuan WangYuxian WangYongbing XieHongbin Cao;
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作者单位

Chemistry & Chemical Engineering Data Center Institute of Process Engineering Chinese Academy of Sciences Beijing 100190, China,University of Chinese Academy of Sciences Beijing 100049, China;

State Key Laboratory of Heavy Oil Processing State Key Laboratory of Petroleum Pollution Control China University of Petroleum-Beijing Beijing 102249, China;

Beijing National Laboratory for Condensed Matter Physics CAS Laboratory of Soft Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190, ChinaChemistry & Chemical Engineering Data Center Institute of Process Engineering Chinese Academy of Sciences Beijing 100190, ChinaChangzheng Engineering Co., Ltd Beijing 101111, China;

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正文语种英语
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catalytic sites; electrons supply; photocatalysis; single-atom catalysts (SACs); surface density;

Surface Density of Cobalt Single Atoms Manipulating Hydroxyl Radical Generation Via Dual Pathways: Electrons Supply and Active sites

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