Abstract Catalysts are essential in the transformation of chemical value chains, and traditional solid catalysts encounter challenges in structural flexibility, interfacial mass transport, and long‐term stability, especially in heterogeneous and electrochemical systems. Liquid metal‐based catalysts, particularly gallium (Ga), provide a dynamic platform with tunable physicochemical properties and favorable interfacial responsiveness. However, the electrochemical interfacial behavior and oxide regulation of Ga‐based liquid metal catalysts in alkaline electrolytes are still largely unexplored. In this work, Pt@Ga is selected as a model system and focused on the alkaline hydrogen evolution reaction (HER) to explore the potential of liquid metal‐based catalysts in the renewable hydrogen energy field. By precisely controlling the Ga surface oxide layer, the in situ formation of Pt wires is enabled with a high proportion of (200) crystal facets. This strategy overcomes the structural constraints of solid supports and enhances the electronic coupling between Pt and Ga. Experimental results from in situ analysis visualize Pt growth dynamics and reveal the synergistic interactions that accelerate charge and mass transport at the catalyst/electrolyte interface. This study presents a novel design for liquid metal‐based catalysts, where oxide‐regulated metal growth and dynamic interface evolution synergistically boost catalyst performance, offering a paradigm for next‐generation self‐adaptive systems.
Chen et al. (Sun,) studied this question.