Single-atom catalysts: Effects of end-group regulation on catalytic activity

被引:2
作者
Wang, Caiqun [1 ,2 ]
Gao, Penglin [2 ]
Li, Hongfei [1 ]
Yang, Mei [3 ]
Jiang, Jun [2 ]
Zhao, Liutao [2 ]
Qian, Ping [1 ]
机构
[1] Univ Sci & Technol Beijing, Dept Phys, Beijing 100083, Peoples R China
[2] Beijing Acad Sci & Technol, Beijing Comp Ctr Co Ltd, Beijing Key Lab Cloud Comp Key Technol & Applicat, Beijing 100094, Peoples R China
[3] Univ Sci & Technol Beijing, Beijing Adv Innovat Ctr Mat Genome Engn, Corros & Protect Ctr, Beijing 100083, Peoples R China
基金
中国国家自然科学基金;
关键词
Monatomic catalyst; CO2RR; Porphyrin-like graphene; End group regulation; CARBON-DIOXIDE; TRANSITION; CO2; ELECTROREDUCTION; REDUCTION; ENERGY;
D O I
10.1016/j.mtcomm.2024.109482
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
The role of 14 metal elements as porphyrin-like monatomic catalysts in carbon dioxide reduction reaction (CO 2 RR) was studied using density functional theory (DFT) and computational hydrogen electrode (CHE) model. It highlights the ability of the catalyst to convert carbon from the + 4 valence state to the + 2 valence state, indicating that the end -tone node significantly improves metal properties and catalytic efficiency. Notably, the modification of the end group improved the structure of the Bi, Sb, and Sn-based catalysts and reduced the free energy barrier, although their initial configuration deviated from the expected configuration. In contrast, Fe, Ti, and V based catalysts showed good initial activity, but performance decreased after the terminal node. In addition, the free energy barrier of Co, Ni, Pd and Ir-based catalysts was significantly reduced by end -group regulation. Detailed analysis of the electron structure, especially Co and Ni, shows that the arrangement of electrons and the localization of d -band electrons through the terminal node are critical for regulating catalyst activity. This study not only highlights the importance of end -tone system in optimizing catalyst performance, but also provides a theoretical basis for designing efficient CO 2 RR catalysts, which is of great significance for the development of sustainable technologies.
引用
收藏
页数:10
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