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231225s2021 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202101741
|2 doi
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|a pubmed24n1092.xml
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|a (DE-627)NLM327659475
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|a (NLM)34219292
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|a DE-627
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|a eng
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|a Xiong, Likun
|e verfasserin
|4 aut
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|a Geometric Modulation of Local CO Flux in AgCu2 O Nanoreactors for Steering the CO2 RR Pathway toward High-Efficacy Methane Production
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|c 2021
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
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|a ƒa Online-Ressource
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|a Date Revised 13.08.2021
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2021 Wiley-VCH GmbH.
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|a 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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|a Journal Article
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|a electrocatalytic CO2 reduction
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|a geometric modulation
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|a methane production
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|a nanocells
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|a oxide-derived copper
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|a Zhang, Xiang
|e verfasserin
|4 aut
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|a Chen, Ling
|e verfasserin
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|a Deng, Zhao
|e verfasserin
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|a Han, Sheng
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|a Chen, Yufeng
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|a Zhong, Jun
|e verfasserin
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|a Sun, Hao
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|a Lian, Yuebin
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|a Yang, Baiyu
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|a Yuan, Xuzhou
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|a Yu, Hui
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|a Liu, Yu
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|a Yang, Xiaoqin
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|a Guo, Jun
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|a Rümmeli, Mark H
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|a Jiao, Yan
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|a Peng, Yang
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 33(2021), 32 vom: 30. Aug., Seite e2101741
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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|g volume:33
|g year:2021
|g number:32
|g day:30
|g month:08
|g pages:e2101741
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|u http://dx.doi.org/10.1002/adma.202101741
|3 Volltext
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