Universal Platform for Robust Dual‐Atom Doped 2D Catalysts with Superior Hydrogen Evolution in Wide pH Media

Abstract Layered 2D transition metal dichalcogenides (TMDs) have been suggested as efficient substitutes for Pt‐group metal electrocatalysts in the hydrogen evolution reaction (HER). However, poor catalytic activities in neutral and alkaline electrolytes considerably hinder their practical applications. Furthermore, the weak adhesion between TMDs and electrodes often impedes long‐term durability and thus requires a binder. Here, a universal platform is reported for robust dual‐atom doped 2D electrocatalysts with superior HER performance over a wide pH range media. V:Co‐ReS₂ on a wafer scale is directly grown on oxidized Ti foil by a liquid‐phase precursor‐assisted approach and subsequently used as highly efficient electrocatalysts. The catalytic performance surpasses that of Pt group metals in a high current regime (≥ 100 mA cm⁻²) at pH ≥ 7, with a high durability of more than 70 h in all media at 200 mA cm⁻². First‐principles calculations reveal that V:Co dual doping in ReS₂ significantly reduces the water dissociation barrier and simultaneously enables the material to achieve the thermoneutral Gibbs free energy for hydrogen adsorption.