Engineering Metal‐Support Interaction for Manipulate Microenvironment: Single‐Atom Platinum Decorated on Nickel‐Chromium Oxides Toward High‐Performance Alkaline Hydrogen Evolution

Abstract Rational construction of platinum (Pt)‐based single‐atom catalysts (SACs) with high utilization of active sites holds promise to achieve superior electrocatalytic alkaline HER performance, which requires the assistance of functional supports. In this work, a novel catalytic configuration is reported, namely, Pt SACs anchored on the nickel‐chromium oxides labeled as Pt SACs‐NiCrO₃/NF. The mechanism associated with the metal‐support interaction (MSI) for synergy co‐catalysis that empowers efficient HER on Pt SACs‐NiCrO₃/NF is clarified. Specifically, the modulated electron structure in Pt SACs‐NiCrO₃ manipulates the interface microenvironment, mediating a more free water state, which is beneficial to accelerate front water dissociation behavior on the oxide support. Besides, the homogeneously distributed Pt sites with the created near‐acidic state ensure the subsequent fast proton‐involved reaction. All these determine the comprehensively accelerating HER kinetics. Consequently, Pt SACs‐NiCrO₃/NF deliverers considerable HER performance, with overpotentials (η₁₀/η₁₀₀) of 23/122 mV, high mass activity of 382.77 mA mg⁻¹_Pt. When serving in an alkaline water‐based anion exchange membrane electrolytic cell (AEMWE), Pt SACs‐NiCrO₃/NF also presents excellent performance (100 mA cm⁻² at the cell voltage of 1.51 V and stable up to 100 h), confirming its good prospect.