Engineering Multifunctional Collaborative Catalytic Interface Enabling Efficient Hydrogen Evolution in All pH Range and Seawater

Abstract Developing electrocatalysts with high compatibility to the reaction systems with complicated chemical properties represents an important frontier of catalyst design. Herein, a strategy by engineering a multifunctional collaborative catalytic interface to propel the hydrogen evolution reaction (HER) in the full pH range and seawater is reported. Collaborative catalytic interfaces among MXene, bimetallic carbide, and hybridized carbon are demonstrated to afford overall enhancement in electrical conductivity, exposure of reactive sites, water dissociation kinetics, H + /water adsorption, and intermediate H binding capability, which satisfy highly variable chemical environment for HER under different pH conditions. Therefore, the HER performance of resultant electrocatalysts can compete with commercial Pt/C in 0.5 m H 2 SO 4 or 1.0 m KOH but outperform it under pH 2.2–11.2. They also show exceptional performance for HER in natural seawater with stringent requirements in catalytic activity and stability, exhibiting the best combination of Pt‐like activity, long durability (225 h, 64 times that of Pt/C), and 98% Faradaic efficiency, comparable with commercial Pt/C and the best documented electrocatalysts by far. This work may shed fresh light into the design of effective electrocatalytic interface for regulating the energy chemistry over wide operation conditions, and also inspires the exploration of hydrogen energy utilization technologies and beyond.