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


研究成果: Article同行評審

273 引文 斯高帕斯(Scopus)


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.

頁(從 - 到)798-803
期刊Angewandte Chemie - International Edition
出版狀態Published - 7 1月 2020


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