Self-Limiting Growth of Single-Layer N-Doped Graphene Encapsulating Nickel Nanoparticles for Efficient Hydrogen Production

Abstract

Effective nonprecious metal catalysts are urgently needed for hydrogen evolution reaction (HER). The hybridization of N-doped graphene and a cost-effective metal is expected to be a promising approach for enhanced HER performance but faces bottlenecks in controllable fabrication. Herein, a silica medium-assisted method is developed for the high-efficient synthesis of single-layer N-doped graphene encapsulating nickel nanoparticles (Ni@SNG), where silica nanosheets molecule sieves tactfully assist the self-limiting growth of single-layer graphene over Ni nanoparticles by depressing the diffusion of gaseous carbon radical reactants. The Ni@SNG sample synthesized at 800 °C shows excellent activity for HER in alkaline medium with a low overpotential of 99.8 mV at 10 mA cm-2, which is close to that of the state-of-the-art Pt/C catalyst. Significantly, the Ni@SNG catalyst is also developed as a binder-free electrode in magnetic field, exhibiting much improved performance than the common Nafion binder-based electrode. Therefore, the magnetism adsorption technique will be a greatly promising approach to overcome the high electron resistance and poor adhesive stability of polymer binder-based electrodes in practical applications. © 2021 American Chemical Society. All rights reserved.