Synergistic Effects of Dual‐Doping with Ni and Ru in Monolayer VS2 Nanosheet: Unleashing Enhanced Performance for Acidic HER through Defects and Strain

Amidst the escalating quest for clean energy, the hydrogen evolution reaction (HER) in acidic conditions has taken center stage, catalyzing the search for advanced electrocatalysts. The efficacy of these materials is predominantly dictated by the active site density on their surfaces. The propensity is leveraged for monolayer architectures to introduce defects, enhancing surface area, and increasing active sites. Doping enhances defects and fine‐tunes catalyst activity. In this vein, defect‐enriched monolayer nanosheets doped with nickel and a trace amount of ruthenium in VS2 (SL‐Ni‐Ru‐VS2) are engineered and characterized. Evaluation in 0.5 m H2SO4 solution unveils that the catalyst achieves overpotentials as low as 20 and 41 mV at current densities of ‐10 and ‐100 mA cm⁻2. Impressively, the catalyst maintains a mass activity of 13.08 A mg⁻¹Ru, even with minimal Ru incorporation, indicating exceptional catalytic efficiency. This monolayer catalyst sustains its high activity at lower overpotentials, demonstrating its practical applicability. The comprehensive analysis, which combines experimental data and computational simulations, indicates that the co‐doping of Ni and Ru enhances the electrocatalytic properties of VS2. This research offers a strategic framework for crafting cutting‐edge electrocatalysts specifically designed for enhanced performance in the HER. Co‐doping Ni and Ru into monolayer VS2 introduces lattice defects and strain, significantly enhancing catalytic activity. The dual role of defects and strain optimizes the electronic structure, provides more active sites, and facilitates charge transfer, demonstrating the potential for precise control of catalyst performance at the nanoscale. This provides valuable insights into the advancement of water electrolysis technology.