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Elucidating the Electrocatalytic CO 2 Reduction Reaction over a Model Single‐Atom Nickel Catalyst

2019; Wiley; Volume: 59; Issue: 2 Linguagem: Inglês

10.1002/anie.201911995

1521-3773

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,

Advanced Photocatalysis Techniques

Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO2 RR) 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 CO2 RR 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 CO2 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 CO2 activation, and functioned as an authentic catalytically active site for the CO2 RR. Furthermore, through combination with a kinetics study, the rate-determining step of the CO2 RR was determined to be *CO2- +H+ →*COOH. This study tackles the four challenges faced by the CO2 RR; namely, activity, selectivity, stability, and dynamics.