期刊
ADVANCED ENERGY MATERIALS
卷 8, 期 31, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201802427
关键词
bimetallic; carbon dioxide reduction; DFT calculations; electrocatalysts; formate
类别
资金
- China Scholarship Council (CSC)
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Waterloo Institute for Nanotechnology
- 111 Project [D17007]
- Henan Center for Outstanding Overseas Scientists of China [GZS2018003]
- University of Waterloo
A highly selective and durable electrocatalyst for carbon dioxide (CO2) conversion to formate is developed, consisting of tin (Sn) nanosheets decorated with bismuth (Bi) nanoparticles. Owing to the formation of active sites through favorable orbital interactions at the Sn-Bi interface, the Bi-Sn bimetallic catalyst converts CO2 to formate with a remarkably high Faradaic efficiency (96%) and production rate (0.74 mmol h(-1) cm(-2)) at -1.1 V versus reversible hydrogen electrode. Additionally, the catalyst maintains its initial efficiency over an unprecedented 100 h of operation. Density functional theory reveals that the addition of Bi nanoparticles upshifts the electron states of Sn away from the Fermi level, allowing the HCOO* intermediate to favorably adsorb onto the Bi-Sn interface compared to a pure Sn surface. This effectively facilitates the flow of electrons to promote selective and durable conversion of CO2 to formate. This study provides sub-atomic level insights and a general methodology for bimetallic catalyst developments and surface engineering for highly selective CO2 electroreduction.
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