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Copper–Nickel Nitride Nanosheets as Efficient Bifunctional Catalysts for Hydrazine‐Assisted Electrolytic Hydrogen Production

Electrocatalytic water splitting is one of the sustainable and promising strategies to generate hydrogen fuel but still remains a great challenge because of the sluggish anodic oxygen evolution reaction (OER). A very effective approach to dramatically decrease the input cell voltage of water electrolysis is to replace the anodic OER with hydrazine oxidation reaction (HzOR) due to its lower thermodynamic oxidation potential. Therefore, developing the low‐cost and efficient HzOR catalysts, coupled with the cathodic hydrogen evolution reaction (HER), is tremendously important for energy‐saving electrolytic hydrogen production. Herein, a new‐type of copper–nickel nitride (Cu1Ni2‐N) with rich Cu4N/Ni3N interface is rationally constructed on carbon fiber cloth. The 3D electrode exhibits extraordinary HER performance with an overpotential of 71.4 mV at 10 mA cm−2 in 1.0 m KOH, simultaneously delivering an ultralow potential of 0.5 mV at 10 mA cm−2 for HzOR in a 1.0 m KOH/0.5 m hydrazine electrolyte. Moreover, the electrolytic cell utilizing the synthesized Cu1Ni2‐N electrode as both the cathode and anode display a cell voltage of 0.24 V at 10 mA cm−2 with an excellent stability over 75 h. The present work develops the promising copper–nickel‐based nitride as a bifunctional electrocatalyst through hydrazine‐assistance for energy‐saving electrolytic hydrogen production.