Electronegativity-assisted optimized electronic structure of functionalized-Pt catalysts for boosting oxygen reduction kinetics

Opportunity to harmonize aspects of oxygen reduction reaction(ORR)performance and structure,and morphology,as well as composition,is urgent for the commercialization of proton exchange membrane fuel cells.Herein,we demonstrate the design and synthesis of a functionalized-supported-Pt catalyst(Pt@HNC)featuring a hollow nitrogen-modified dodecahedral carbon substrate obtained by a stress-induced-shrink tailoring route.The as-obtained Pt@HNC catalyst possesses enhanced ORR per-formance,in particular with half-wave potential,mass activity(MA)and specific activity,which greatly exceed the commercial Pt/C.The density functional theory(DFT)calculations further confirmed that the charge redistribution induced by the electronegativity differences improved the electron interaction between Pt and HNC support.The optimized electronic structure of Pt weakens the reaction energy barrier on the Pt@HNC surface and adsorption of^(*)OH species,thus cooperatively improving the intrinsic activity toward ORR.Additionally,our work indeed provides a guide for the future design of functional nanomaterials in the field of catalysts and clean energy.