Electrochemical conversion of carbon dioxide (electrochemical reduction of carbon dioxide) to value‐added products is a promising way to solve CO2 emission problems. This paper describes a facile one‐pot approach to synthesize palladium–copper (Pd–Cu) bimetallic catalysts with different structures. Highly efficient performance and tunable product distributions are achieved due to a coordinative function of both enriched low‐coordinated sites and composition effects. The concave rhombic dodecahedral Cu3Pd (CRD‐Cu3Pd) decreases the onset potential for methane (CH4) by 200 mV and shows a sevenfold CH4 current density at −1.2 V (vs reversible hydrogen electrode) compared to Cu foil. The flower‐like Pd3Cu (FL‐Pd3Cu) exhibits high faradaic efficiency toward CO in a wide potential range from −0.7 to −1.3 V, and reaches a fourfold CO current density at −1.3 V compared to commercial Pd black. Tafel plots and density functional theory calculations suggest that both the introduction of high‐index facets and alloying contribute to the enhanced CH4 current of CRD‐Cu3Pd, while the alloy effect is responsible for high CO selectivity of FL‐Pd3Cu.
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Small 2018, 14, 1703314 (Cover Story)