Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts
- Ruhr Univ., Bochum (Germany). Dept. of Physics; Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics
- Ruhr Univ., Bochum (Germany). Dept. of Physics
- Copenhagen Univ. (Denmark). Dept. of Chemistry
- Univ. of Pittsburgh, PA (United States). Chemical and Petroleum Engineering and Physics
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Univ. of Copenhagen (Denmark). Dept. of Chemistry
- Ruhr Univ., Bochum (Germany). Dept. of Physics; Fritz-Haber Inst. of the Max Planck Society, Berlin (Germany). Dept. of Interface Science
Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO2 is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO2 electroreduction to CO. At -0.6 V versus RHE more than 90 % Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. Finally, DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO2 electroreduction.
- Research Organization:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE
- Grant/Contract Number:
- SC0012704; AC02-06CH11357; FG02-03ER15476; CHEM 1213182; CHE-1534630; 03SF0523C; ERC-725915; CF15-0165
- OSTI ID:
- 1433976
- Alternate ID(s):
- OSTI ID: 1374678
- Report Number(s):
- BNL-203511-2018-JAAM
- Journal Information:
- Angewandte Chemie (International Edition), Vol. 56, Issue 38; ISSN 1433-7851
- Publisher:
- WileyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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