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

Authors: Hemma Mistry, Yong-Wook Choi, Alexander Bagger, Fabian Scholten, Cecile Bonifacio, Ilya Sinev, Nuria J. Divins, Ioannis Zegkinoglou, Hyo Sang Jeon, Kim Kisslinger, Eric A. Stach, Judith C. Yang, Jan Rossmeisl, Beatriz Roldan Cuenya

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.

Comments: 46 Pages. Angewandte Chemie 2017

Download: PDF

Submission history

[v1] 2018-05-11 07:01:50

Unique-IP document downloads: 5 times is a pre-print repository rather than a journal. Articles hosted may not yet have been verified by peer-review and should be treated as preliminary. In particular, anything that appears to include financial or legal advice or proposed medical treatments should be treated with due caution. will not be responsible for any consequences of actions that result from any form of use of any documents on this website.

Add your own feedback and questions here:
You are equally welcome to be positive or negative about any paper but please be polite. If you are being critical you must mention at least one specific error, otherwise your comment will be deleted as unhelpful.

comments powered by Disqus