Molybdenum Sulfide Nanosheets Coupled with Ni2P Hollow Microspheres as an Efficient Electrocatalyst for Hydrogen Generation over a Wide pH Range Mediated by a 3D/2D Interface

Abstract Developing high activity, strong durability, and cost‐efficient electrocatalysts for the hydrogen evolution reaction (HER) is critical for the sustainable production of hydrogen energy. Herein, we have rationally designed three‐dimensional (3D) heterogeneous catalyst of hollow nickel phosphide spheres coupled with molybdenum sulfide nanosheets (Ni 2 P@MoS 2 ). Benefiting from the hollow spherical structure and the coupling effects between MoS 2 and Ni 2 P, Ni 2 P@MoS 2 shows superior activity for hydrogen generation over a wide pH range. It displays overpotentials of 181, 269 and 535 mV in 1.0 M KOH, 0.5 M H 2 SO 4 and 1.0 M PBS, respectively, at a current density of 10 mA cm −2 . A series of characterization techniques demonstrate that the strong coupling interaction between Ni 2 P and MoS 2 effectively optimizes the electronic structure of the Ni 2 P‐MoS 2 3D/2D interfaces, beneficial for regulating H* adsorption energy. This work offers a novel strategy for enhancing the HER performance of metal phosphide/sulfide catalysts by constructing heterostructured materials with abundant 3D/2D interfaces.