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Customizing CO2 Electroreduction by Pulse-Induced Anion Enrichment.

Jianghao Wang1,2, Yanyang Qin3, Shoutong Jin1

  • 1School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China.

Journal of the American Chemical Society
|November 9, 2023
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Summary

Anion enrichment via pulsed electrolysis controls copper-catalyzed carbon dioxide electroreduction (CO2RR). This strategy tunes product selectivity towards CO, C2+ products, or methane (CH4) by altering electrolyte composition.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Electrochemical conversion of carbon dioxide (CO2) to valuable products is crucial for carbon-neutral economies.
  • Controlling product distribution in CO2 electroreduction using copper-based catalysts remains a significant challenge.
  • Tuning catalyst selectivity is key to efficient CO2 utilization.

Purpose of the Study:

  • To develop an anion enrichment strategy for controlling CO2 electroreduction product selectivity.
  • To investigate the effect of pulsed electrolysis and electrolyte composition on CO2 electroreduction pathways.
  • To understand the mechanism by which enriched anions influence CO2 reduction intermediates.

Main Methods:

  • Pulsed electrolysis strategy applied to commercial copper foil electrodes.
  • Systematic variation of electrolyte composition (KF, KCl, KHCO3) to achieve anion enrichment.
  • Product analysis to determine selectivity for CO, C2+ products, and methane (CH4).
  • Density functional theory (DFT) calculations to elucidate reaction mechanisms.

Main Results:

  • Pulsed electrolysis with anion enrichment successfully tuned CO2 electroreduction products.
  • Specific electrolytes yielded high selectivity for CO (53% ± 2.5 with KF), C2+ (76.6 ± 2.1% with KCl), and CH4 (42.6 ± 2.1% with KHCO3).
  • The ratios of CO/CH4, CH4/C2+, and C2+/CO could be precisely controlled by electrolyte modification.
  • DFT calculations confirmed that anion properties (electronegativity, volume) influence key intermediates and selectivity.

Conclusions:

  • Anion enrichment is an effective strategy for controlling CO2 electroreduction product distribution on copper catalysts.
  • Pulsed electrolysis provides a method to manipulate the interfacial ionic environment for tailored catalysis.
  • This approach offers a pathway for customizing CO2 electroreduction products by tuning electrolyte composition.