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Elucidating the Electrocatalytic CO 2 Reduction Reaction over a Model Single‐Atom Nickel Catalyst
Author(s) -
Liu Song,
Yang Hong Bin,
Hung SungFu,
Ding Jie,
Cai Weizheng,
Liu Linghui,
Gao Jiajian,
Li Xuning,
Ren Xinyi,
Kuang Zhichong,
Huang Yanqiang,
Zhang Tao,
Liu Bin
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201911995
Subject(s) - nickel , catalysis , electrocatalyst , raman spectroscopy , x ray photoelectron spectroscopy , electrochemical reduction of carbon dioxide , electrochemistry , carbon fibers , chemistry , reaction mechanism , materials science , photochemistry , inorganic chemistry , chemical engineering , electrode , carbon monoxide , organic chemistry , physics , composite number , composite material , optics , engineering
Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO 2 RR) is an appealing approach to tackling the challenges posed by rising CO 2 levels and realizing a closed carbon cycle. However, fundamental understanding of the complicated CO 2 RR mechanism in CO 2 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‐N 4 moiety on a conductive carbon support with which to explore the electrochemical CO 2 RR. 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 CO 2 activation, and functioned as an authentic catalytically active site for the CO 2 RR. Furthermore, through combination with a kinetics study, the rate‐determining step of the CO 2 RR was determined to be *CO 2 − +H + →*COOH. This study tackles the four challenges faced by the CO 2 RR; namely, activity, selectivity, stability, and dynamics.