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*, Xu Lu*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

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.

Original languageEnglish (US)
Article number2958
JournalNature communications
Volume14
Issue number1
DOIs
StatePublished - Dec 2023

ASJC Scopus subject areas

  • General Chemistry
  • General Biochemistry, Genetics and Molecular Biology
  • General Physics and Astronomy

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