Efficient wettability-controlled electroreduction of CO2 to CO at Au/C interfaces

Run Shi, Jiahao Guo, Xuerui Zhang, Geoffrey I. N. Waterhouse, Zhaojun Han, Yunxuan Zhao, Lu Shang, Chao Zhou, Lei Jiang and Tierui Zhang ()
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Run Shi: Chinese Academy of Sciences
Jiahao Guo: Chinese Academy of Sciences
Xuerui Zhang: Chinese Academy of Sciences
Geoffrey I. N. Waterhouse: The University of Auckland
Zhaojun Han: CSIRO Manufacturing
Yunxuan Zhao: Chinese Academy of Sciences
Lu Shang: Chinese Academy of Sciences
Chao Zhou: Chinese Academy of Sciences
Lei Jiang: Chinese Academy of Sciences
Tierui Zhang: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract The electrochemical CO2 reduction reaction (CO2RR) represents a very promising future strategy for synthesizing carbon-containing chemicals in a more sustainable way. In spite of great progress in electrocatalyst design over the last decade, the critical role of wettability-controlled interfacial structures for CO2RR remains largely unexplored. Here, we systematically modify the structure of gas-liquid-solid interfaces over a typical Au/C gas diffusion electrode through wettability modification to reveal its contribution to interfacial CO2 transportation and electroreduction. Based on confocal laser scanning microscopy measurements, the Cassie-Wenzel coexistence state is demonstrated to be the ideal three phase structure for continuous CO2 supply from gas phase to Au active sites at high current densities. The pivotal role of interfacial structure for the stabilization of the interfacial CO2 concentration during CO2RR is quantitatively analysed through a newly-developed in-situ fluorescence electrochemical spectroscopic method, pinpointing the necessary CO2 mass transfer conditions for CO2RR operation at high current densities.

Date: 2020
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DOI: 10.1038/s41467-020-16847-9

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