Hierarchical SiC-Graphene Composite Aerogel-Supported Ni-Mo-S Nanosheets for Efficient pH-Universal Electrocatalytic Hydrogen Evolution.

Abstract

MoS2 exhibits good prospects in electrocatalytic hydrogen evolution. Whereas, the electrocatalytic property of MoS2 is restrained by its insufficient active sites, low electrical conductivity, and slow water dissociation processes. Herein, an aerogel composed of silicon carbide (SiC) and graphene (SiCnw-RGO) was constructed by growing SiC nanowires (SiCnw) in the graphene aerogel (RGO) via the CVD method, and then Ni-Mo-S nanosheets were hydrothermally synthesized on the SiCnw-RGO composite aerogel to develop an efficient pH-universal electrocatalyst. Ni-Mo-S nanosheets supported on SiCnw-RGO (Ni-Mo-S@SiCnw-RGO) exhibit an interesting hierarchical three-dimensional interconnected structure of composite aerogel. The optimal Ni-Mo-S@SiCnw-RGO electrocatalyst exhibits excellent catalytic performance with low Tafel slopes of 60 mV/dec under acidic conditions and 90 mV/dec under alkaline conditions. Density functional theory calculations demonstrate a composite catalyst exhibits advantageous hydrogen adsorption free energy and water dissociation energy barrier. This study provides a reference to design an efficient hierarchical aerogel electrocatalyst.