Materializing Efficient Collaborative Multifunctional Electrocatalysis via the Electron Delocalization Effect between Pt and Substrate

Investigating multifunctional electrocatalysts is essential for advancing energy storage and conversion technologies. Herein, we report a hybrid composite catalyst (Pt@Co/NC) in which Pt nanoparticles (NPs) are uniformly implanted into porous Co- and N-codoped carbon spheres. The unique porous structure and charge-transfer-induced electron delocalization of Pt@Co/NC significantly enhance its electrocatalytic activity. Enhanced stability and anti-CO poisoning are also observed, attributed to surface spatial confinement and an optimized electronic structure. Moreover, Pt@Co/NC-based zinc-air batteries exhibit superior open-circuit potential and power density. The Extended X-ray Absorption Fine Structure analysis shows a relatively prominent peak at ∼1.58 Å, which is attributed to the contribution of Pt–N bonds, indicating the electronic delocalization effect between Pt and the Co/NC substrate. Density Functional Theory further determines that the d-band center of Pt is regulated by the electron delocalization effect between Pt and Co–N4 sites, promoting efficient *CO to CO2 conversion and *OH desorption on the Pt surface, achieving efficient collaborative multifunctional electrocatalysis.