Electrochemical small-molecule oxidation-boosted water electrolysis has proven to be an energy-saving strategy for electrochemical hydrogen (H2) production. Herein, trimetallic RhNiFe phosphide nanosheets on nickel foam (RhNiFe-P/NF) with high electrocatalytic activity are synthesized for constructing a bifunctional electrocatalyst toward the hydrogen evolution reaction (HER) and ethanol oxidation reaction (EOR). Ultrathin RhNiFe-P nanosheets vertically grow on the surface of the three-dimensional (3D) nickel network, and the thickness of the RhNiFe-P nanosheets is only 1.5 nm. The introduction of Rh atoms in RhNiFe-P/NF can regulate the electronic structure and reduce adsorption energy to elevate the electrocatalytic activity. Benefiting from the excellent bifunctional electrocatalytic property of RhNiFe-P/NF, the corresponding two-electrode ethanol device displays a low cell voltage (1.42 V), smaller than that of traditional devices on water electrolysis (1.61 V) at 10 mA cm–2. Meanwhile, electrochemical reforming of ethanol can decrease catalytic voltage in H2 production and generate highly valuable potassium acetate as a byproduct.

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