Unraveling the rate-determining step of C2+ products during electrochemical CO reduction

Wanyu Deng, Peng Zhang, Yu Qiao, Georg Kastlunger, Nitish Govindarajan, Aoni Xu, Ib Chorkendorff, Brian Seger () and Jinlong Gong ()
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Wanyu Deng: Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Peng Zhang: Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Yu Qiao: Technical University of Denmark
Georg Kastlunger: Technical University of Denmark
Nitish Govindarajan: Technical University of Denmark
Aoni Xu: Technical University of Denmark
Ib Chorkendorff: Technical University of Denmark
Brian Seger: Technical University of Denmark
Jinlong Gong: Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract The electrochemical reduction of CO has drawn a large amount of attention due to its potential to produce sustainable fuels and chemicals by using renewable energy. However, the reaction’s mechanism is not yet well understood. A major debate is whether the rate-determining step for the generation of multi-carbon products is C-C coupling or CO hydrogenation. This paper conducts an experimental analysis of the rate-determining step, exploring pH dependency, kinetic isotope effects, and the impact of CO partial pressure on multi-carbon product activity. Results reveal constant multi-carbon product activity with pH or electrolyte deuteration changes, and CO partial pressure data aligns with the theoretical formula derived from *CO-*CO coupling as the rate-determining step. These findings establish the dimerization of two *CO as the rate-determining step for multi-carbon product formation. Extending the study to commercial copper nanoparticles and oxide-derived copper catalysts shows their rate-determining step also involves *CO-*CO coupling. This investigation provides vital kinetic data and a theoretical foundation for enhancing multi-carbon product production.

Date: 2024
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DOI: 10.1038/s41467-024-45230-1

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