Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 10, Issue 10, Pages 8574-8584Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b15418
Keywords
electrochemical CO2 reduction; CO adsorption; chronopotentiometry; Raman spectroscopy; Cu2O reduction; DFT modeling
Funding
- Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) program through the Singapore-Berkeley Research Initiative for Sustainable Energy (SinBeRISE)
- NUSNNI-Nanocore
- Centre for Advanced 2D Materials - National Research Foundation, Prime Minister's Office, Singapore, under its Medium Size Centre program
- academic research grant from National University of Singapore [R-143-000-683-112]
- Ministry of Education, Singapore
- Air Force Office of Scientific Research Grant [FA9550-17-0198]
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Copper oxides have been of considerable interest as electrocatalysts for CO2 reduction (CO2R) in aqueous electrolytes. However, their role as an active catalyst in reducing the required overpotential and improving the selectivity of reaction compared with that of polycrystalline copper remains controversial. Here, we introduce the use of selected-ion flow tube mass spectrometry, in concert with chronopotentiometry, in situ Raman spectroscopy, and computational modeling, to investigate CO2R on Cu2O nanoneedles, Cu2O nanocrystals, and Cu(2)0 nanoparticles. We show experimentally that the selective formation of gaseous C-2 products (i.e., ethylene) in CO2R is preceded by the reduction of the copper oxide (Cu2OR) surface to metallic copper. On the basis of density functional theory modeling, CO2R products are not formed as long as Cu2O is present at the surface because Cu2OR is kinetically and energetically more favorable than CO2R.
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