期刊
ACS CATALYSIS
卷 8, 期 6, 页码 4996-5001出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b00365
关键词
gold nanoclusters; atomic precision; morphology; CO2 electroreduction
资金
- Air Force Office of Scientific Research under AFOSR Award [FA9550-15-1-9999, FA9550-15-1-0154]
- National Science Foundation (NSF, CBET-CAREER program) [1652694]
- NSF Graduate Research Fellowship [1247842]
- NSF [ACI-1548562]
- NSF DMREF [CHE-1534630]
Gold-based materials hold promise in electrocatalytic reduction of CO2 to fuels. However, the polydispersity of conventional gold nanostructures limits mechanistic studies. Here, we report two types of atomically precise Au-25 nanoclusters (1 nm) with distinct morphology (i.e., nanosphere and nanorod) for CO2 reduction catalysis. The Au-25 nanosphere exhibits higher Faradaic efficiency for CO with higher formation rates compared to the Au-25 nanorod. First-principles calculations reveal that the negative charge and the energetically favorable removal of one ligand to generate an active site on the nanosphere can better stabilize the important *COOH intermediate in CO2 electroreduction.
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