摘要: Nickel-cobalt (NiCo) alloys with bimetallic electronic modulation are considered promising candidates for urea electrolysis. However, their highly occupied d-band states limit the adsorption of reaction intermediates, resulting in insufficient activity toward urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). Herein, a phosphorus-doped amorphous NiCo alloy is synthesized, in which P incorporation modulates the electronic structure and upshifts the d-band center of NiCo alloy, thus optimizing the adsorption of OH− and urea molecules. The sample with optimal P content exhibits low potentials for UOR (E10/1000 = 1.28/1.65 VRHE) and HER (E−10/−1000 = −67/−206 mVRHE). Furthermore, it achieves an industrial-level current density of 500 mA cm−2 at a cell voltage of 1.72 V in the membrane electrode assembly, while maintaining stable activity for 150 h. Therefore, this work provides a new strategy to optimize reactant adsorption and ultimately enhance the electrocatalytic activity by modulating the d-band center.