Zinc‐Coordinated Nitrogen‐Codoped Graphene as an Efficient Catalyst for Selective Electrochemical Reduction of CO2 to CO

• Published in: ChemSusChem Vol. 11; no. 17; pp. 2944 - 2952
• Main Authors: Chen, Zhipeng, Mou, Kaiwen, Yao, Shunyu, Liu, Licheng
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 11.09.2018
• Subjects: active sites; Carbon dioxide; Carbon monoxide; Catalysis; Catalysts; Chemical reduction; electrocatalysis; Fine structure; Graphene; Nitrogen; Organic chemistry; reduction; Zinc
• ISSN: 1864-5631; 1864-564X
• DOI: 10.1002/cssc.201800925

Electrochemical reduction of CO2 to value‐added chemicals by using renewable electricity offers a promising strategy to deal with rising CO2 emission and the energy crisis. Single‐site zinc‐coordinated nitrogen‐codoped graphene (Zn–N–G) catalyzes the electrochemical reduction of CO2 to CO. The Zn–N–G catalyst exhibits excellent intrinsic activity toward CO2 reduction, reaching a faradaic efficiency of 91 % for CO production at a low overpotential of 0.39 V. X‐ray absorption fine structure and X‐ray photoelectron spectroscopy both confirm the presence of isolated Zn–Nx moieties, which act as the key active sites for CO formation. DFT calculations reveal the origin of enhanced activity for CO2 reduction on Zn–N–G catalysts. This work provide further understanding of the active centers on transition metal–nitrogen–carbon (M–N–C) catalysts for electrochemical reduction of CO2 to CO. What a site! Single‐site zinc‐coordinated nitrogen‐codoped graphene catalysts for highly selective electrochemical reduction of CO2 to CO were prepared by consecutive pyrolysis and acid leaching. A maximum CO faradaic efficiency of 91 % was attained with high stability at a low overpotential of 390 mV.