Elucidating the Electrocatalytic CO2 Reduction Reaction over a Model Single-Atom Nickel Catalyst

Song Liu, Hong Bin Yang, Sung Fu Hung, Jie Ding, Weizheng Cai, Linghui Liu, Jiajian Gao, Xuning Li, Xinyi Ren, Zhichong Kuang, Yanqiang Huang*, Tao Zhang, Bin Liu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

199 Scopus citations

Abstract

Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO2RR) is an appealing approach to tackling the challenges posed by rising CO2 levels and realizing a closed carbon cycle. However, fundamental understanding of the complicated CO2RR mechanism in CO2 electrocatalysis is still lacking because model systems are limited. We have designed a model nickel single-atom catalyst (Ni SAC) with a uniform structure and well-defined Ni-N4 moiety on a conductive carbon support with which to explore the electrochemical CO2RR. Operando X-ray absorption near-edge structure spectroscopy, Raman spectroscopy, and near-ambient X-ray photoelectron spectroscopy, revealed that Ni+ in the Ni SAC was highly active for CO2 activation, and functioned as an authentic catalytically active site for the CO2RR. Furthermore, through combination with a kinetics study, the rate-determining step of the CO2RR was determined to be *CO2 +H+→*COOH. This study tackles the four challenges faced by the CO2RR; namely, activity, selectivity, stability, and dynamics.

Original languageEnglish
Pages (from-to)798-803
Number of pages6
JournalAngewandte Chemie - International Edition
Volume59
Issue number2
DOIs
StatePublished - 7 Jan 2020

Keywords

  • Active site
  • Electrochemistry
  • In situ reactions
  • Reaction mechanisms
  • Single-atom catalysts

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