A Strongly Coupled Cluster Heterostructure with Pt–N-Mo Bonding for Durable and Efficient H2 Evolution in Anion-Exchange Membrane Water Electrolyzers

Abstract Creating strongly coupled heterostructures with favorable catalytic activities is crucial for promoting the performance of catalytic reactions, especially those involve multiple intermediates. Herein, we fabricated a strongly coupled platinum/molybdenum nitrides nanocluster heterostructure on nitrogen-doped reduced graphene oxide (Pt/Mo₂N–NrGO) for alkaline hydrogen evolution reaction. The well-defined Pt-containing Anderson-type polyoxometalates promote strong interfacial Pt–N–Mo bonding in Pt/Mo 2 N–NrGO, which exhibits a remarkably low overpotential, high mass activity, and exceptional long-term durability (> 500 h at 1500 mA cm⁻ 2 ) in an anion-exchange membrane water electrolyzer (AEMWE). Operando Raman spectroscopy and density functional theory reveal that pronounced electronic coupling at the Pt/Mo₂N cluster interface facilitates the catalytic decomposition of H 2 O through synergistic stabilization of intermediates (Pt–H* and Mo-OH*), thereby enhancing the kinetics of the rate-determining Volmer step. Techno-economic analysis indicates a levelized hydrogen production cost of $2.02 kg⁻ 1 , meeting the US DOE targets. Our strategy presents a viable pathway to designing next-generation catalysts for industrial AEMWE for green hydrogen production.