Microwave-assisted CVD-like synthesis of dispersed monolayer/few-layer N-doped graphene encapsulated metal nanocrystals for efficient electrocatalytic oxygen evolution

Abstract

Herein a novel and general microwave-assisted chemical vapor deposition (CVD)-like synthetic strategy was developed to realize the ultrafast synthesis of a series of well-dispersed monolayer/few-layer N-doped graphene shell encapsulated metal nanocrystals (M@NC) by using a metal–organic framework (MOF) on graphene as precursors for the first time. Unlike traditional programmed heat treatment, this microwave-assisted method decomposed the MOF into separated metal and carbon- and nitrogen-containing gases rather than aggregated metal and carbon composites during the initial thermal transformation stages. This change ensured the effective control of the subsequent formation process of carbon on the surface of metal and led to the formation of well-dispersed M@NC with monolayer/few-layer NC. Moreover, the graphene substrate promoted the full exposure of all active monolayer/few-layer NC, and thus the obtained FeNi@NC/graphene displays the best electrocatalytic properties for the oxygen evolution reaction of all of the previously reported M@NC based catalysts, including the lowest overpotential (261 mV) at 10 mA cm⁻² in alkaline electrolyte (1 M KOH), the smallest Tafel slope (40 mV dec⁻¹) and excellent durability for at least 120 h.