Exploring the highly active and stable nonprecious metal electrocatalysts is particularly important for the advancement of water electrolysis, whereas it remains a challenge to efficiently improve the intrinsic electrocatalytic activity. Herein, we reasonably constructed a self-supporting nanosheet array material with sulfur incorporated into WP2. Because of the tunability of electronic configuration and the formation of partial metal phase sulfides, the optimized catalyst exhibits a low overpotential of 115 mV at 10 mA cm-2, along with superb durability over 24 h in acidic media. Furthermore, theoretical calculations reveal that sulfur substitution effectively manipulates the local electronic configuration of WP2, which reduces the interaction between the catalyst surface and hydrogen atoms, thus improving the intrinsic activity of the hydrogen evolution reaction. This work provides valuable insight into the rational fabrication of highly efficient flexible electrode materials based on resourceful electrocatalysts for electrochemical water splitting.
Keywords: hydrogen evolution reaction; nanosheet arrays; sulfur incorporation; tungsten diphosphide; tuning electronic structure.