Abstract

Water electrolysis is an environmentally-friendly strategy for hydrogen production but suffers from significant energy consumption. Substituting urea oxidation reaction (UOR) with lower theoretical voltage for water oxidation reaction adopting nickel-based electrocatalysts engenders reduced energy consumption for hydrogen production. The main obstacle remains strong interaction between accumulated Ni3+ and *COO in the conventional Ni3+-catalyzing pathway. Herein, a novel Ni3+/Ni2+ mediated pathway for UOR via constructing a heterojunction of nickel metaphosphate and nickel telluride (Ni2P4O12/NiTe), which efficiently lowers the energy barrier of UOR and avoids the accumulation of Ni3+ and excessive adsorption of *COO on the electrocatalysts, is developed. As a result, Ni2P4O12/NiTe demonstrates an exceptionally low potential of 1.313V to achieve a current density of 10mA cm-2 toward efficient urea oxidation reaction while simultaneously showcases an overpotential of merely 24mV at 10mA cm-2 for hydrogen evolution reaction. Constructing urea electrolysis electrolyzer using Ni2P4O12/NiTe at both sides attains 100mA cm-2 at a low cell voltage of 1.475V along with excellent stability over 500 h accompanied with nearly 100% Faradic efficiency.

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