Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction

Hong Bin Yang, Sung-Fu Hung, Song Liu, Kaidi Yuan, Shu Miao, Liping Zhang, Xiang Huang, Hsin-Yi Wang, Weizheng Cai, Rong Chen, Jiajian Gao, Xiaofeng Yang, Wei Chen, Yanqiang Huang (), Hao Ming Chen, Chang Ming Li, Tao Zhang () and Bin Liu ()
Additional contact information
Hong Bin Yang: Nanyang Technological University
Sung-Fu Hung: National Taiwan University
Song Liu: Nanyang Technological University
Kaidi Yuan: National University of Singapore
Shu Miao: Chinese Academy of Sciences
Liping Zhang: Nanyang Technological University
Xiang Huang: Nanyang Technological University
Hsin-Yi Wang: Nanyang Technological University
Weizheng Cai: Nanyang Technological University
Rong Chen: Nanyang Technological University
Jiajian Gao: Nanyang Technological University
Xiaofeng Yang: Chinese Academy of Sciences
Wei Chen: National University of Singapore
Yanqiang Huang: Chinese Academy of Sciences
Hao Ming Chen: National Taiwan University
Chang Ming Li: Suzhou University of Science and Technology
Tao Zhang: Chinese Academy of Sciences
Bin Liu: Nanyang Technological University

Nature Energy, 2018, vol. 3, issue 2, 140-147

Abstract: Abstract Electrochemical reduction of CO2 to chemical fuel offers a promising strategy for managing the global carbon balance, but presents challenges for chemistry due to the lack of effective electrocatalyst. Here we report atomically dispersed nickel on nitrogenated graphene as an efficient and durable electrocatalyst for CO2 reduction. Based on operando X-ray absorption and photoelectron spectroscopy measurements, the monovalent Ni(i) atomic center with a d9 electronic configuration was identified as the catalytically active site. The single-Ni-atom catalyst exhibits high intrinsic CO2 reduction activity, reaching a specific current of 350 A gcatalyst−1 and turnover frequency of 14,800 h−1 at a mild overpotential of 0.61 V for CO conversion with 97% Faradaic efficiency. The catalyst maintained 98% of its initial activity after 100 h of continuous reaction at CO formation current densities as high as 22 mA cm−2.

Date: 2018
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DOI: 10.1038/s41560-017-0078-8

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