Revealing Correlation-driven Charge transfer and Electron Redistribution via strong metal-metal interactions in the Construction of High Stability Pt Catalysts

Developing catalysts with high performance for the oxygen reduction reaction via a cost-effective methodology is the key to promoting the industrialization of fuel cells. Herein, we design and synthesize a Pt-Mo 2 C/NC dual-composite with a unique electronic coupling interface, where the electronic structure and surface property of Pt can be precisely controlled by using the macro-porous cross-linked anion exchange resin as a chelating agent via a facile “in-situ concurrent pyrolysis-reduction” route. The XAFS analysis reveals that each Pt atom in the Pt-Mo 2 C/NC dual-composite catalyst coordinates with ~1.29 N atoms, ~5.88 Pt atoms and ~1.81 Mo atoms, respectively. Moreover, DFT calculations further confirm the strong interfacial coupling effect between metal Pt and Mo 2 C support, resulting in the formation of electron-rich regions at the Pt-Mo interface, which can act as an “electronic reservoir” and optimize the adsorption energy of the ORR intermediate. Benefiting from the constructed electron-enriched region and the induced strong interfacial coupling effect, the obtained Pt-Mo 2 C/NC catalyst exhibits enhanced ORR electrocatalysis activity, with a mass activity and specific activity of 0.65 A/mg Pt and 1.16 mA/cm 2 . Such an efficient synthesis of high-performance Pt-Mo 2 C/NC nanocomposite with controlled particle size and composition is extremely desired in energy conversion materials.