Enhanced Electroreduction of Carbon Dioxide to Methanol using Zinc Dendrites Pulse‐deposited on Silver Foam

The electroreduction of CO2 (CO2RR) can dynamize the carbon cycle by lowering anthropogenic CO2 emissions and sustainably producing valuable fuels and chemical feedstock. Methanol is arguably the most desirable C1 product of CO2RR, although it typically forms in negligible amounts. In our search for efficient methanol‐producing CO2RR catalysts, we engineer Ag‐Zn catalysts by pulse‐depositing Zn dendrites on Ag foams (PD‐Zn/Ag foam). By themselves, Zn and Ag cannot effectively reduce CO2 to CH3OH, while their alloys gave CH3OH with Faradaic efficiencies (FE) of ~1%. Interestingly, with nanostructuring, PD‐Zn/Ag foam reduces CO2 to CH3OH with FE and current densities reaching as high as 10.5% and ‐2.7mA/cm2, respectively. Control experiments and DFT calculations pinpoint strained undercoordinated Zn atoms as the active sites for CO2RR to CH3OH in a reaction pathway mediated by adsorbed CO and formaldehyde. Surprisingly, the stability of the *CHO intermediate does not influence the activity.

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