Pressure dependence in aqueous-based electrochemical CO2 reduction

Liang Huang, Ge Gao, Chaobo Yang, Xiao-Yan Li, Rui Kai Miao, Yanrong Xue, Ke Xie, Pengfei Ou, Cafer T. Yavuz, Yu Han, Gaetano Magnotti (), David Sinton (), Edward H. Sargent () and Xu Lu ()
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Liang Huang: King Abdullah University of Science and Technology (KAUST)
Ge Gao: King Abdullah University of Science and Technology (KAUST)
Chaobo Yang: King Abdullah University of Science and Technology (KAUST)
Xiao-Yan Li: University of Toronto
Rui Kai Miao: University of Toronto
Yanrong Xue: King Abdullah University of Science and Technology (KAUST)
Ke Xie: University of Toronto
Pengfei Ou: University of Toronto
Cafer T. Yavuz: Advanced Membranes and Porous Materials Center (AMPM), PSE, KAUST
Yu Han: Advanced Membranes and Porous Materials Center (AMPM), PSE, KAUST
Gaetano Magnotti: King Abdullah University of Science and Technology (KAUST)
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto
Xu Lu: King Abdullah University of Science and Technology (KAUST)

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Electrochemical CO2 reduction (CO2R) is an approach to closing the carbon cycle for chemical synthesis. To date, the field has focused on the electrolysis of ambient pressure CO2. However, industrial CO2 is pressurized—in capture, transport and storage—and is often in dissolved form. Here, we find that pressurization to 50 bar steers CO2R pathways toward formate, something seen across widely-employed CO2R catalysts. By developing operando methods compatible with high pressures, including quantitative operando Raman spectroscopy, we link the high formate selectivity to increased CO2 coverage on the cathode surface. The interplay of theory and experiments validates the mechanism, and guides us to functionalize the surface of a Cu cathode with a proton-resistant layer to further the pressure-mediated selectivity effect. This work illustrates the value of industrial CO2 sources as the starting feedstock for sustainable chemical synthesis.

Date: 2023
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DOI: 10.1038/s41467-023-38775-0

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