Geometric modulation of local CO Flux in Ag@Cu₂ O nanoreactors for steering the CO₂ RR pathway toward high-efficacy methane production
Date
2021
Authors
Xiong, L.
Zhang, X.
Chen, L.
Deng, Z.
Han, S.
Chen, Y.
Zhong, J.
Sun, H.
Lian, Y.
Yang, B.
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Journal article
Citation
Advanced Materials, 2021; 33(32):e2101741-1-e2101741-11
Statement of Responsibility
Likun Xiong, Xiang Zhang, Ling Chen, Zhao Deng, Sheng Han, Yufeng Chen ... et al.
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Abstract
The electroreduction of carbon dioxide (CO2 RR) to CH4 stands as one of the promising paths for resourceful CO2 utilization in meeting the imminent "carbon-neutral" goal of the near future. Yet, limited success has been witnessed in the development of high-efficiency catalysts imparting satisfactory methane selectivity at a commercially viable current density. Herein, a unique category of CO2 RR catalysts is fabricated with the yolk-shell nanocell structure, comprising an Ag core and a Cu2 O shell that resembles the tandem nanoreactor. By fixing the Ag core and tuning the Cu2 O envelope size, the CO flux arriving at the oxide-derived Cu shell can be regulated, which further modulates the *CO coverage and *H adsorption at the Cu surface, consequently steering the CO2 RR pathway. Density functional theory simulations show that lower CO coverage favors methane formation via stabilizing the intermediate *CHO. As a result, the best catalyst in the flow cell shows a high CH4 Faraday efficiency of 74 ± 2% and partial current density of 178 ± 5 mA cm- 2 at -1.2 VRHE , ranking above the state-of-the-art catalysts reported today for methane production. These findings mark the significance of precision synthesis in tailoring the catalyst geometry for achieving desired CO2 RR performance.
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© 2021 Wiley-VCH GmbH