期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 2, 页码 798-803出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201911995
关键词
Active site; Electrochemistry; In situ reactions; Reaction mechanisms; Single-atom catalysts
资金
- National Key R&D Program of China [2016YFB0600902]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Dalian National Laboratory for Clean Energy [DNL180401]
- Youth Innovation Promotion Association CAS
- Singapore Ministry of Education Academic Research Fund (AcRF) [RG9/17, RG115/17, RG115/18, MOE2016-T2-2-004]
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-N-4 moiety on a conductive carbon support with which to explore the electrochemical CO2RR. Operando X-ray absorption nearedge 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.
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