期刊
ACS CATALYSIS
卷 7, 期 8, 页码 5431-5437出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b01548
关键词
CO2 conversion; Cu/CuxO catalysts; electro-catalysis; hydrocarbon formation; metal sponge
资金
- CTI Swiss Competence Center for Energy Research (SCCER Heat and Electricity Storage)
- Swiss National Foundation [200020_172507]
- interfaculty Microscopy Imaging Centre (MIC) of the University of Bern
- Swiss National Science Foundation (SNF) [200020_172507] Funding Source: Swiss National Science Foundation (SNF)
Highly porous 3D Cu skeletons (sponges) modified by electropolishing, thermal annealing, and foam electrodeposition have been studied as catalysts for the electrochemical conversion of CO2 with a particular emphasis on C-2 products formation. These catalyst materials appear to be promising for future applications where gaseous CO2 reactants can be transported through the 3D catalyst thereby tuning the mean residence time of reaction intermediates inside the catalyst, which crucially influences the final product distribution. In particular, the annealed skeleton (300 degrees C, 12 h) and the one modified by Cu foam electrodeposition show profound activities toward C-2 product formation (C2H4, C2H6) with faradaic efficiencies reaching FEC2 = 32.3% (annealed skeleton sample, -1.1 V vs RHE) and FEC2 = 29.1% (electrodeposited sample, -1.1 V vs RHE), whereas the electropolished Cu skeleton remains largely inactive for both the C-1 and the C-2 pathway of hydrocarbon formation. This effect is discussed on the basis of residual impurities that are left behind from the investment casting approach on which the fabrication of these Cu skeleton support materials is based. In addition, a higher FEC2H4/FEC2H6 ratio is observed for the annealed Cu skeleton as compared to the electrodeposited Cu foam. Such a switching in the C-2 product distribution (FEC2H4/FEC2H6 ratio) is discussed on the basis of particular morphological effects (residence time of intermediates inside the catalyst) related to the three-dimensional nature of the used catalysts.
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