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Optimizing Electron Densities of Ni‐N‐C Complexes by Hybrid Coordination for Efficient Electrocatalytic CO 2 Reduction
Author(s) -
Wang ZhongLi,
Choi Jaecheol,
Xu Mingquan,
Hao Xianfeng,
Zhang Hao,
Jiang Zheng,
Zuo Ming,
Kim Jeonghun,
Zhou Wu,
Meng Xianguang,
Yu Qing,
Sun Zhihu,
Wei Shiqiang,
Ye Jinhua,
Wallace Gordon G.,
Officer David L.,
Yamauchi Yusuke
Publication year - 2020
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201903427
Subject(s) - electrocatalyst , reduction (mathematics) , electron , electrochemistry , nickel , chemistry , coordination complex , materials science , inorganic chemistry , electrode , metallurgy , physics , metal , mathematics , geometry , quantum mechanics
Metal‐N‐C is a type of attractive electrocatalyst for efficient CO 2 reduction to CO. Because of the ambiguity in their atomic structures, the active sites and catalytic mechanisms of the catalysts have remained under debate. Here, the effects of N and C hybrid coordination on the activity of Ni‐N‐C catalysts were investigated, combining theoretical and experimental methods. The theoretical calculations revealed that N and C hybrid coordination greatly enhanced the capability of single‐atom Ni active sites to provide electrons to reactant molecules and strengthens the bonding of Ni to N and C in the Ni‐N‐C complexes. During the reaction process, the C and N coordination synergistically optimized the reaction energies in the conversion of CO 2 to CO. A good agreement between theoretical calculations and electrochemical experiments was achieved based on the newly developed Ni‐N‐C electrocatalysts. The activity of hybrid‐coordination NiN 2 C 2 was more than double that of single‐coordination NiN 4 .