Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts.

Autor: Mistry H; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany.; Department of Physics, University of Central Florida, Orlando, FL, 32816, USA., Choi YW; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany., Bagger A; Department of Chemistry, University of Copenhagen, Copenhagen, Denmark., Scholten F; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany., Bonifacio CS; Chemical and Petroleum Engineering and Physics, University of Pittsburgh, Pittsburgh, PA, 15261, USA., Sinev I; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany., Divins NJ; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany., Zegkinoglou I; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany., Jeon HS; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany., Kisslinger K; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York, 11973, USA., Stach EA; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York, 11973, USA., Yang JC; Chemical and Petroleum Engineering and Physics, University of Pittsburgh, Pittsburgh, PA, 15261, USA., Rossmeisl J; Department of Chemistry, University of Copenhagen, Copenhagen, Denmark., Roldan Cuenya B; Department of Physics, Ruhr University Bochum, 44780, Bochum, Germany.; Department of Interface Science, Fritz-Haber Institute of the Max Planck Society, 14195, Berlin, Germany.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2017 Sep 11; Vol. 56 (38), pp. 11394-11398. Date of Electronic Publication: 2017 Aug 10.
DOI: 10.1002/anie.201704613
Abstrakt: Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO 2 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 CO 2 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. 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 CO 2 electroreduction.
(© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)
Databáze: MEDLINE
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