期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 3, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202113498
关键词
C-C coupling; CO2 electroreduction; Diffusion kinetics; Nanoconfinement
资金
- National Key Research and Development Program of China [2019YFA0405600]
- National Science Fund for Distinguished Young Scholars [21925204]
- NSFC [U19A2015, 22005291, 22102018, 52171201]
- Fundamental Research Funds for the Central Universities
- Provincial Key Research and Development Program of Anhui [202004a05020074]
- USTC Research Funds of the Double First-Class Initiative [YD2340002002]
- University of Electronic Science and Technology of China (UESTC) [A1098531023601264]
The research found that Cu HoMSs structure has a high selectivity for C2+ products in CO2 electroreduction, and the C2+ Faradaic efficiency increases with the increase in shell numbers. Mechanistic studies show that superposition of Cu shells in HoMSs structure can increase the coverage of CO adsorbate, promoting carbon dimerization.
Nanoconfinement provides a promising solution to promote electrocatalytic C-C coupling, by dramatically altering the diffusion kinetics to ensure a high local concentration of C-1 intermediates for carbon dimerization. Herein, under the guidance of finite-element method simulations results, a series of Cu2O hollow multi-shell structures (HoMSs) with tunable shell numbers were synthesized via Ostwald ripening. When applied in CO2 electroreduction (CO2RR), the in situ formed Cu HoMSs showed a positive correlation between shell numbers and selectivity for C2+ products, reaching a maximum C2+ Faradaic efficiency of 77.0 +/- 0.3 % at a conversion rate of 513.7 +/- 0.7 mA cm(-2) in a neutral electrolyte. Mechanistic studies clarified the confinement effect of HoMSs that superposition of Cu shells leads to a higher coverage of localized CO adsorbate inside the cavity for enhanced dimerization. This work provides valuable insights for the delicate design of efficient C-C coupling catalysts.
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