The development of efficient, stable and low‐cost electrocatalysts for hydrogen evolution reaction (HER) through a facile strategy is undoubtedly vital to realize sustainable production of H2 in water splitting but still challenging. Herein, we present a one‐step approach, a simultaneous phosphorization and sulfurization thermal treatment of NF at low temperature, to direct grow Ni‐S−P heteronanorod arrays consisting of Ni3S2 and Ni2P on nickel foam (Ni‐S−P NRs/NF). Due to the direct growth, one‐dimensional structure and good conductivity of the catalyst hybrid, as well as the synergistic effect between Ni3S2 and Ni2P, the resultant Ni‐S−P NRs/NF exhibited excellent HER electrocatalytic activity over a wide pH range. Ni‐S−P NRs/NF shows an overpotential of 180, 148 and 292 mV to reach the current density of 100 mA cm−2 in 1.0 M KOH, 0.5 M H2SO4 and 1.0 M PBS solution, respectively. DFT theoretical calculations was further confirmed that the superior pH‐universal HER activity of Ni‐S−P NRs/NF is originated from the thermo‐neutral hydrogen adsorption free energy and the enhanced adsorption of water molecular by the Ni3S2/Ni2P heterostructure.
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