The Effect of the 3D Nanoarchitecture and Ni-Promotion on the Hydrogen Evolution Reaction in MoS2 /Reduced GO Aerogel Hybrid Microspheres Produced by a Simple One-Pot Electrospraying Procedure

Abstract

The transition toward renewable energy sources requires low-cost, efficient, and durable electrocatalysts for green H₂ production. Herein, an easy and highly scalable method to prepare MoS₂ nanoparticles embedded in 3D partially reduced (pr) graphene oxide (GO) aerogel microspheres (MoS₂ /prGOAMs) with controlled morphology and composition is described. Given their peculiar center-diverging mesoporous structure, which allows easy access to the active sites and optimal mass transport, and their efficient electron transfer facilitated by the intimate contact between the MoS₂ and the 3D connected highly conductive pr-GO sheets, these materials exhibit a remarkable electrocatalytic activity in the hydrogen evolution reaction (HER). Ni atoms, either as single Ni atoms or NiO aggregates are then introduced in the MoS₂ /prGOAMs hybrids, to facilitate water dissociation, which is the slowest step in alkaline HER, producing a bifunctional catalyst. After optimization, Ni-promoted MoS₂ /prGOAMs obtained at 500 °C reach a remarkable η₁₀ (overpotential at 10 mA cm^-2 ) of 160 mV in 1 m KOH and 174 mV in 0.5 m H₂ SO₄ . Moreover, after chronopotentiometry tests (15 h) at a current density of 10 mA cm^-2 , the η₁₀ value improves to 147 mV in alkaline conditions, indicating an exceptional stability.

Keywords: 2D materials; Ni-promotion; hybrid materials; hydrogen evolution reaction; mesoporous materials.