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https://hdl.handle.net/2440/131458
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Type: | Journal article |
Title: | Geometric modulation of local CO Flux in Ag@Cu₂ O nanoreactors for steering the CO₂ RR pathway toward high-efficacy methane production |
Other Titles: | Geometric modulation of local CO Flux in Ag@Cu(2) O nanoreactors for steering the CO(2) RR pathway toward high-efficacy methane production |
Author: | Xiong, L. Zhang, X. Chen, L. Deng, Z. Han, S. Chen, Y. Zhong, J. Sun, H. Lian, Y. Yang, B. Yuan, X. Yu, H. Liu, Y. Yang, X. Guo, J. Rümmeli, M.H. Jiao, Y. Peng, Y. |
Citation: | Advanced Materials, 2021; 33(32):e2101741-1-e2101741-11 |
Publisher: | Wiley |
Issue Date: | 2021 |
ISSN: | 0935-9648 1521-4095 |
Statement of Responsibility: | Likun Xiong, Xiang Zhang, Ling Chen, Zhao Deng, Sheng Han, Yufeng Chen ... et al. |
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. |
Keywords: | electrocatalytic CO
2 reduction geometric modulation methane production nanocells oxide-derived copper |
Rights: | © 2021 Wiley-VCH GmbH |
DOI: | 10.1002/adma.202101741 |
Grant ID: | http://purl.org/au-research/grants/arc/FT190100636 |
Published version: | http://dx.doi.org/10.1002/adma.202101741 |
Appears in Collections: | Aurora harvest 8 Physics publications |
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