Agglomeration-triggered deactivation of supported platinum electrocatalysts markedly hinders their application in methanol oxidation reaction (MOR). In this study, graphene-supported nickel–iron layered double hydroxide (NiFe-LDH/rGO), in which Fe3+ was introduced to replace Ni2+ partially in the Ni(OH)2 lattice to provide stronger metal–support bonding sites, was utilized to immobilize Pt nanoparticles (NPs). Given the optimized metal–support interfacial contact (Fe3+-O(H)-Pt) between Pt NPs and NiFe-LDH/rGO nanosheets for Pt/NiFe-LDH/rGO electrocatalysts, the Pt/NiFe-LDH/rGO electrocatalysts displayed dramatically enhanced durability than that of Pt/Ni(OH)2/rGO counterpart as well as commercial Pt/C, and 86.5% of its initial catalytic activity can be maintained even after 1200 cycles of cyclic voltammetry (CV) tests during MOR. First-principle calculations toward the resultant M-O(H)-Pt (M = Fe3+, Ni2+) interfacial structure further corroborates that the NiFe-LDH nanosheets can provide stronger bonding sites (via the Fe3+-O(H)-Pt bonds) to immobilize Pt NPs than those of Ni(OH)2 nanosheets (via the Ni2+-O(H)-Pt bonds).

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