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学術論文

Enhanced carbon dioxide electroreduction to carbon monoxide over defect rich plasma‐activated silver catalysts

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Roldan Cuenya, Beatriz
Interface Science, Fritz Haber Institute, Max Planck Society;

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引用

Mistry, H., Choi, Y.-W., Bagger, A., Scholten, F., Bonifacio, C., Sinev, I., Divins, N. J., Zegkinoglou, I., Jeon, H. S., Kisslinger, K., Stach, E. A., Yang, J. C., Rossmeisl, J., & Roldan Cuenya, B. (2017). Enhanced carbon dioxide electroreduction to carbon monoxide over defect rich plasma‐activated silver catalysts. Angewandte Chemie International Edition. doi:10.1002/anie.201704613.

要旨

Efficient, stable catalysts with high selectivity for a single product are essential to making the electroreduction of CO₂ a viable route to the synthesis of industrial feedstocks and fuels. We reveal how a plasma oxidation pre-treatment can lead to an enhanced content of low-coordinated active sites which dramatically lower the overpotential and increase the activity of CO₂ electroreduction to CO. At -0.6 V vs. RHE, more than 90% Faradaic efficiency towards CO could be achieved on a pre-oxidized silver foil. While transmission electron microscopy 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 show how the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields results in a drastic decrease in the overpotential for the electroreduction of CO₂.