Surface-Regulated Platinum–Copper Nanoframes in Electrochemical Reforming of Ethanol for Efficient Hydrogen Production

Replacing the kinetics sluggish oxygen evolution reaction with thermodynamically favorable ethanol oxidation reaction (EOR) is a prospective method to boost energy-efficient hydrogen production. Surface regulation has achieved great success in enhancing catalytic performance, but it has been rarely demonstrated for the coupled hydrogen evolution reaction (HER)/EOR to date. Herein, the three-dimensional PtCu nanoframe (NF) with high-index facets and multi-channels is designed through a dealloying strategy to achieve bifunctional catalysis for HER and EOR. The PtCu NF/C needs only 0.58 V to arrive at 10 mA cm–2 in the coupled HER/EOR, while 1.88 V is required in water splitting. Moreover, ethanol can be oxidized by PtCu NF/C to acetate with a high Faradaic efficiency of 92%. Mechanistic studies reveal that the combination of the three-dimensional structure, Cu introduction, and high-index facets endows the PtCu NF/C with enhanced adsorption capacity for ethanol and H2O, as well as dissociation capacity for C–H bonds of ethanol. This work is the icing on the cake for bifunctional electrocatalysts and the further development of energy-saving hydrogen evolution.