Single-Atom Molybdenum Engineered Platinum Nanocatalyst for Boosted Alkaline Hydrogen Oxidation

摘要

Engineering the surface electrochemistry at the atomic level can precisely and effectively manipulate the reactivity and durability of catalysts. Herein, a novel single-atom fine-tailoring strategy based on a highly hydrophilic Mo-bifunctional promoter is proposed to greatly boost the hydrogen oxidation reaction (HOR) on Pt catalysts. The single-atom Mo-modified nanometer Pt anchored on porous N-doped carbon (Mo-Pt/NC) is developed via a pyrolysis-adsorption-reduction process. The designed Mo-Pt/NC exhibits a remarkable mass-specific kinetic current reaching 1584 mA mg(Pt)(-1) in 0.1 m KOH, which is nearly 11-fold and fourfold higher than the activities of commercial Pt/C and Pt/NC counterparts respectively, and such extraordinary HOR behavior even exceeds those of documented Pt-related catalysts. Electrochemical and spectroscopic studies indicate that hydrophilic Mo single-atom sites can not only regulate the electronic microenvironment of Pt sites for attenuated H* adsorption, but they also serve as energetic H2O*-adsorption promoters to jointly facilitate the HOR kinetics. Moreover, the anti-CO poisoning capability of Mo-Pt/NC is markedly enhanced by this Mo-modified electronic effect. This work gives a significant guideline for the design of high-performance HOR catalysts and other advanced catalysts.