Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides

Electrochemical CO2 reduction reaction (CO2RR) with renewable electricity is a potentially sustainable method to reduce CO2 emissions. Palladium supported on cost‐effective transition‐metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO2RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO2RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO2RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low‐cost and stable substrates to support and modify Pd for enhanced CO2RR activity. Transitional metal carbide (TMC) substrates are shown to play an important role in tuning the activity and selectivity of electrochemical reduction of CO2 (CO2RR) by adjusting the surface properties. This study provides a promising prospect for using TMCs as low‐cost substrates to develop cost‐effective and efficient electrocatalysts.