Atomically Dispersed Platinum Sites Immobilized on NiFe LDH by Controlling Localized Amorphization for Efficient Alkaline Electrocatalytic Hydrogen Evolution

Platinum (Pt) single‐atom catalyst (SAC) shows great promise for hydrogen evolution reaction (HER), but faces a huge challenge in activity enhancement due to the isolated single‐atom sites. Fabricating support with partially amorphous (pa) structures to realize the synergetic interaction in neighboring single atoms could facilitate H 2 O dissociation and optimize H* adsorption. However, the electrocatalytic mechanism of SAC achieved by tailoring the different amorphous contents of the support has not been clearly explored yet. Herein, neighboring Pt SAs confined in NiFe LDH (Pt@pa‐NiFe LDH‐24) were successfully synthesized via a localized amorphization and impregnation strategy, resulting in significantly boosted HER performance. Experiments and calculations demonstrate that the Pt SAs can accelerate the adsorption/desorption of H 2 O and effectively promote the Volmer step of the partially amorphous substrate. Benefiting from this, the optimized Pt@pa‐NiFe LDH‐24 exhibits enhanced intrinsic activity, exhibiting a lower overpotential ( η 10 : 40 mV) than the commercial Pt/C catalyst. This partial amorphization strategy sheds new light on supporting noble metal single‐atom catalysts for designing efficient HER catalysts in water electrolysis.