Site-specifically Immobilize Pt Nanocrystals on NiFe Layered Double Hydroxide: Old Catalysts with Enhanced Stability Through strong Fe3+-O(H)-Pt Interfacial Contact

摘要: 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).