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, Bin Liu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

522 Scopus citations

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 d 9 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.

Original languageEnglish
Pages (from-to)140-147
Number of pages8
JournalNature Energy
Volume3
Issue number2
DOIs
StatePublished - 1 Feb 2018

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