Molten salt‐mediated enhancement of bimetallic synergy for highly efficient hydrogen evolution across a wide <scp>pH</scp> range

Abstract Constructing bimetallic synergy is key to enhancing the hydrogen evolution reaction (HER), yet simultaneously tailoring active‐site morphology and inducing strong coupling under mild conditions remains challenging. Here, we introduce a facile molten‐salt mediating approach that reconstructs ruthenium clusters on nickel foam into hexagonal‐like nanostructures and strengthens Ru–Ni interfacial coupling. The resultant catalyst delivers 500 mA cm −2 at low overpotentials of 144 mV in 0.5 M H 2 SO 4 and 166 mV in 1.0 M KOH, and sustains 50 mA cm −2 for over 500 h in both acidic and alkaline electrolytes, even in corrosive 3.0 M H 2 SO 4 . Experimental and theoretical analyses, including H 2 ‐TPD, XAFS, quasi in‐situ XPS, and DFT calculations, reveal that the molten‐salt environment facilitates Ni incorporation into the Ru lattice, tuning electronic states and optimizing hydrogen adsorption/desorption kinetics. This work establishes a general pathway integrating nanostructure engineering with bimetallic synergy for high‐performance electrocatalyst design.