Promoting CO2 Electroreduction Kinetics on Atomically Dispersed Monovalent ZnI Sites by Rationally Engineering Proton-Feeding Centers
Jiayi Chen
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Search for more papers by this authorDr. Zhongjian Li
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorXinyue Wang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Search for more papers by this authorProf. Dr. Xiahan Sang
Nanostructure Research Center, Wuhan University of Technology, Wuhan, 430070 China
Search for more papers by this authorSixing Zheng
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Search for more papers by this authorProf. Dr. Shoujie Liu
Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031 China
Search for more papers by this authorDr. Bin Yang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorProf. Dr. Qinghua Zhang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorProf. Dr. Lecheng Lei
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorProf. Dr. Liming Dai
Australian Carbon Materials Centre(A-CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052 Australia
Search for more papers by this authorCorresponding Author
Prof. Dr. Yang Hou
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorJiayi Chen
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Search for more papers by this authorDr. Zhongjian Li
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorXinyue Wang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Search for more papers by this authorProf. Dr. Xiahan Sang
Nanostructure Research Center, Wuhan University of Technology, Wuhan, 430070 China
Search for more papers by this authorSixing Zheng
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Search for more papers by this authorProf. Dr. Shoujie Liu
Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031 China
Search for more papers by this authorDr. Bin Yang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorProf. Dr. Qinghua Zhang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorProf. Dr. Lecheng Lei
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorProf. Dr. Liming Dai
Australian Carbon Materials Centre(A-CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052 Australia
Search for more papers by this authorCorresponding Author
Prof. Dr. Yang Hou
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
Institute of Zhejiang University—Quzhou, Quzhou, 324000 China
Search for more papers by this authorAbstract
Electrocatalytic reduction of CO2 (CO2RR) to value-added chemicals is of great significance for CO2 utilization, however the CO2RR process involving multi-electron and proton transfer is greatly limited by poor selectivity and low yield. Herein, We have developed an atomically dispersed monovalent zinc catalyst anchored on nitrogenated carbon nanosheets (Zn/NC NSs). Benefiting from the unique coordination environment and atomic dispersion, the Zn/NC NSs exhibit a superior CO2RR performance, featuring a high current density up to 50 mA cm−2 with an outstanding CO Faradaic efficiency of ≈95 %. The center ZnI atom coordinated with three N atoms and one N atom that bridges over two adjacent graphitic edges (Zn-N3+1) is identified as the catalytically active site. Experimental results reveal that the twisted Zn-N3+1 structure accelerates CO2 activation and protonation in the rate-determining step of *CO2 to *COOH, while theoretical calculations elucidate that atomically dispersed Zn-N3+1 moieties decrease the potential barriers for intermediate COOH* formation, promoting the proton-coupled CO2RR kinetics and boosting the overall catalytic performance.
Conflict of interest
The authors declare no conflict of interest.
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