Geometric Modulation of Local CO Flux in AgCu2 O Nanoreactors for Steering the CO2 RR Pathway toward High-Efficacy Methane Production

Geometric Modulation of Local CO Flux in AgCu2 O Nanoreactors for Steering the CO2 RR Pathway toward High-Efficacy Methane Production

© 2021 Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 32 vom: 30. Aug., Seite e2101741
1. Verfasser: Xiong, Likun (VerfasserIn)
Weitere Verfasser: Zhang, Xiang, Chen, Ling, Deng, Zhao, Han, Sheng, Chen, Yufeng, Zhong, Jun, Sun, Hao, Lian, Yuebin, Yang, Baiyu, Yuan, Xuzhou, Yu, Hui, Liu, Yu, Yang, Xiaoqin, Guo, Jun, Rümmeli, Mark H, Jiao, Yan, Peng, Yang
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2021
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article electrocatalytic CO2 reduction geometric modulation methane production nanocells oxide-derived copper
Beschreibung
Zusammenfassung:© 2021 Wiley-VCH GmbH.
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
Beschreibung:Date Revised 13.08.2021
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202101741