Atomically Dispersed Platinum Supported on Crumpled Graphene Supports for Highly Efficient Hydrogen Evolution Reaction

Platinum (Pt) single‐atom catalysts (SACs) are a promising alternative to commercial Pt/carbon (C) catalysts because of their tunable catalytic activity with maximum atomic efficiency for the hydrogen evolution reaction (HER). Herein, we report a nitrogen (N)‐doped three‐dimensional (3D) crumpled graphene‐supported Pt SAC (NCG/Pt) that efficiently catalyzes HER under acidic media. The NCG/Pt demonstrates an overpotential of 0.11 V at a current density of 10 mA cm −2 with a mass activity of 2852.9 A g −1 Pt , highlighting its superior 3.6 times greater hydrogen (H) production capacity compared to Pt/C. Systematically controlled electrochemical characterization together with synchrotron‐based X‐ray absorption spectroscopy (XAS) and N 2 adsorption–desorption isotherm experiment successfully established the structure–activity relationship, and the enhanced catalytic performance was mainly attributed to the synergistic effect between the Pt‐pyridinic N 4 moiety and the crumpled graphene (CG) support. Our work presents a rational approach to designing a highly effective, robust, and efficient electrocatalyst for acidic HER.