A high throughput optical method for studying compositional effects in electrocatalysts for CO2 reduction

Jeremy L. Hitt, Yuguang C. Li, Songsheng Tao, Zhifei Yan, Yue Gao, Simon J. L. Billinge and Thomas E. Mallouk ()
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Jeremy L. Hitt: The University of Pennsylvania
Yuguang C. Li: University at Buffalo, The State University of New York
Songsheng Tao: Columbia University
Zhifei Yan: The University of Pennsylvania
Yue Gao: The Pennsylvania State University, University Park
Simon J. L. Billinge: Columbia University
Thomas E. Mallouk: The University of Pennsylvania

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract In the problem of electrochemical CO2 reduction, the discovery of earth-abundant, efficient, and selective catalysts is essential to enabling technology that can contribute to a carbon-neutral energy cycle. In this study, we adapt an optical high throughput screening method to study multi-metallic catalysts for CO2 electroreduction. We demonstrate the utility of the method by constructing catalytic activity maps of different alloyed elements and use X-ray scattering analysis by the atomic pair distribution function (PDF) method to gain insight into the structures of the most active compositions. Among combinations of four elements (Au, Ag, Cu, Zn), Au6Ag2Cu2 and Au4Zn3Cu3 were identified as the most active compositions in their respective ternaries. These ternary electrocatalysts were more active than any binary combination, and a ca. 5-fold increase in current density at potentials of −0.4 to −0.8 V vs. RHE was obtained for the best ternary catalysts relative to Au prepared by the same method. Tafel plots of electrochemical data for CO2 reduction and hydrogen evolution indicate that the ternary catalysts, despite their higher surface area, are poorer catalysts for the hydrogen evolution reaction than pure Au. This results in high Faradaic efficiency for CO2 reduction to CO.

Date: 2021
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DOI: 10.1038/s41467-021-21342-w

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