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Proton-Transfer Dynamics Regulates CO2 Electroreduction Products via Hydrogen Coverage.

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This study regulates electrochemical reduction of carbon dioxide (CO2) to hydrocarbons by tuning proton transfer rates with a resin layer. This method controls product selectivity, offering insights into carbon neutrality and energy storage solutions.

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Area of Science:

  • Electrochemistry
  • Catalysis
  • Materials Science

Background:

  • Electrochemical conversion of CO2 to hydrocarbons is key for carbon neutrality and energy storage.
  • Understanding proton transfer is crucial for controlling CO2 reduction (CO2RR) product selectivity and reaction mechanisms.

Purpose of the Study:

  • To develop a strategy for regulating CO2RR product selectivities by tuning local proton transport rates.
  • To investigate the influence of proton transfer rates on product selectivity using a surface resin layer over cuprous oxides.

Main Methods:

  • Systematic study of resorcinol-formaldehyde (RF) resin polymerization degree to control proton transfer rates.
  • Electrochemical experiments and theoretical calculations to analyze the effect of the resin layer on CO2RR.
  • Tuning local proton transport rates via a surface resin layer over cuprous oxides.

Main Results:

  • The RF resin layer effectively regulated local proton transfer rates.
  • Product selectivity between C2 compounds and methane (CH4) was switched by altering the RF coating.
  • A maximum CH4 Faradaic efficiency of 51% was achieved at amperage-level current densities.
  • The resin layer influenced hydrogen coverage on catalytic sites, guiding electrochemical performance.

Conclusions:

  • Surface resin layers can precisely tune proton transfer rates in CO2RR.
  • This strategy offers a method to control product selectivity for CO2 electrochemical reduction.
  • The findings provide insights into the catalytic mechanisms of CO2RR and pathways to carbon neutrality.