Selectivity

Ionic liquid

Nanotechnology

Electrode

Organic chemistry

Electrocatalyst

Engineering

Faraday efficiency

Catalysis

Physical chemistry

Inorganic chemistry

Chemistry

Materials science

Methanol

Tetrafluoroborate

Electrolyte

Chemical engineering

Electrochemistry

Nature Communications

Methanol is a highly desirable product of CO2 electroreduction due to its wide array of industrial applications. However, the development of CO2-to-methanol electrocatalysts with high performance is still challenging. Here we report an operationally simple in situ dual doping strategy to construct efficient CO2-to-methanol electrocatalysts. In particular, when using Ag,S-Cu2O/Cu as electrocatalyst, the methanol Faradaic efficiency (FE) could reach 67.4% with a current density as high as 122.7 mA cm-2 in an H-type cell using 1-butyl-3-methylimidazolium tetrafluoroborate/H2O as the electrolyte, while the current density was below 50 mA cm-2 when the FE was greater than 50% over the reported catalysts. Experimental and theoretical studies suggest that the anion S can effectively adjust the electronic structure and morphology of the catalysts in favor of the methanol pathway, whereas the cation Ag suppresses the hydrogen evolution reaction. Their synergistic interactions with host material enhance the selectivity and current density for methanol formation. This work opens a way for designing efficient catalysts for CO2 electroreduction to methanol.

In situ dual doping for constructing efficient CO2-to-methanol electrocatalysts