Journal
SCIENCE CHINA-CHEMISTRY
Volume 63, Issue 12, Pages 1727-1733Publisher
SCIENCE PRESS
DOI: 10.1007/s11426-020-9847-9
Keywords
carbon dioxide reduction; electrochemical; electron-withdrawing; cobalt phthalocyanine; single-atom
Categories
Funding
- 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]
- National Natural Science Foundation of China [21925803]
- Young Scholar Training Program of Jilin University
- Singapore Ministry of Education [RG9/17, RG115/17, RG115/18, MOE2016-T2-2-004]
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Electrochemical carbon dioxide reduction reaction (CO2RR) powered by renewable electricity offers an attractive approach to reduce carbon emission and at the same time produce valuable chemicals/fuels. To design efficient CO2 reduction electrocatalyst, it is important to understand the structure-activity relationship. Herein, we design a series of single Co atoms electrocatalysts with well-defined active sites electronic structures, which exhibit outstanding CO2RR activity with controllable selectivity to CO. Experimental and density functional theory (DFT) calculation studies show that introducing nitro (amino) ligand next to single Co atom catalytic center with electron-withdrawing (electron-donating) capability favors (hinders) CO2 reduction catalysis. This work provides an in-depth understanding of how functional ligand affects the splitting of transition metal 3d electron orbital, thereby changing the electron transfer from transition metal active site to CO2, which is closely related to the Gibbs free energy of the rate-determining step (CO2+e(-)+*->*CO2-).
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