Strong Fe-O(H)-Pt Interfacial Interaction Induced Excellent Stability of Pt/NiFe-LDH/rGO Electrocatalysts.

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 Fe was introduced to replace Ni partially in the Ni(OH) lattice to provide stronger metal-support bonding sites, was utilized to immobilize Pt nanoparticles (NPs). Given the optimized metal-support interfacial contact (Fe-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)/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 = Fe, Ni) interfacial structure further corroborates that the NiFe-LDH nanosheets can provide stronger bonding sites (via the Fe-O(H)-Pt bonds) to immobilize Pt NPs than those of Ni(OH) nanosheets (via the Ni-O(H)-Pt bonds).