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

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/MoN-NrGO, which exhibits a remarkably low overpotential, high mass activity, and exceptional long-term durability (> 500 h at 1500 mA cm⁻) 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 HO 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⁻, meeting the US DOE targets. Our strategy presents a viable pathway to designing next-generation catalysts for industrial AEMWE for green hydrogen production.