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

Hemma Mistry, Yong-Wook Choi, Alexander Bagger, Fabian Scholten, Cecile S Bonifacio, Ilya Sinev, Nuria J Divins, Ioannis Zegkinoglou, Hyo Sang Jeon, Kim Kisslinger, Eric A Stach, Judith C Yang, Jan Rossmeisl, Beatriz Roldan Cuenya
Angewandte Chemie 2017 September 11, 56 (38): 11394-11398
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. 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.

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