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

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.