Optimizing Electron Densities of Ni-N-C Complexes by Hybrid Coordination for Efficient Electrocatalytic CO2 Reduction

Zhong Li Wang, Jaecheol Choi, Mingquan Xu, Xianfeng Hao, Hao Zhang, Zheng Jiang, Ming Zuo, Jeonghun Kim, Wu Zhou, Xianguang Meng, Qing Yu, Zhihu Sun, Shiqiang Wei, Jinhua Ye, Gordon G. Wallace, David L. Officer, Yusuke Yamauchi

Research output: Contribution to journalArticlepeer-review

21 Citations (Scopus)

Abstract

Metal-N-C is a type of attractive electrocatalyst for efficient CO2 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 CO2 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 NiN2C2 was more than double that of single-coordination NiN4.

Original languageEnglish
Pages (from-to)929-937
Number of pages9
JournalChemSusChem
Volume13
Issue number5
DOIs
Publication statusPublished - 2020 Mar 9

Bibliographical note

Funding Information:
This research was partially supported by the Grant-in-Aid for International Research Fellow of the Japan Society for the Promotion of Science (JSPS), the Natural Science Foundation of China (51622211), the Key Research Program of the CAS (XDPB08-1), the ARC Center of Excellence Scheme (Project Number CE 140100012), and Foundation for Australia-Japan Studies Grant. The authors thank beamline BL14W1 of Shanghai Synchrotron Radiation Facility for the beam time. This work was performed in part at the Queensland node of the Australian National Fabrication Facility (ANFF), a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia?s researchers.

Funding Information:
This research was partially supported by the Grant‐in‐Aid for International Research Fellow of the Japan Society for the Promotion of Science (JSPS), the Natural Science Foundation of China (51622211), the Key Research Program of the CAS (XDPB08‐1), the ARC Center of Excellence Scheme (Project Number CE 140100012), and Foundation for Australia‐Japan Studies Grant. The authors thank beamline BL14W1 of Shanghai Synchrotron Radiation Facility for the beam time. This work was performed in part at the Queensland node of the Australian National Fabrication Facility (ANFF), a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia′s researchers.

Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

All Science Journal Classification (ASJC) codes

  • Environmental Chemistry
  • Chemical Engineering(all)
  • Materials Science(all)
  • Energy(all)

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