Publication date: 15th December 2025
Two-dimensional (2D) molybdenum sulfide (MoS2) is an attractive noble-metal-free electrocatalyst for the hydrogen evolution (HER) in acids. Tremendous effort has been made to engineer MoS2 catalysts with either more active sites or higher conductivities to enhance their HER activity. However, little attention has been paid to structural and electronic modulations of MoS2 synergistically. Moreover, the Hads energies for most of MoS2 based catalysts have not been well-clarified so far.
Herein, 2D hydrogenated graphene (HG) was introduced as the support of MoS2 nanosheets for the construction of MoS2/HG hybrid catalysts. The optimized MoS2/HG hybrid catalysts characterized using scanning microscopy and transmission electron microscopy showed that vertical MoS2 ultrathin nansheets arrays are highly ordered and uniformly distributed on the surface of HG. Wrinkled MoS2 nanosheets are interconnected with each other, leading to the formation of a porous structure. The characteristic bonds of C-Mo were observed in Raman spectrum. These unique structure characteristics make vertically aligned MoS2 nanosheets feature more accessible catalytic active sites and ultrafast electron transfer from the HG substrate to the MoS2 edges within one S-Mo-S layer.
To gain further the idea about the electronic structures of MoS2 on HG and the Hads energy of the optimized hybrid catalysts, Density Functional Theory (DFT) calculations were conducted. The simulation results confirmed the improvement of the content of Hads on MoS2 by the adequate ferromagnetism of HG support as well as the optimized electronic structure (the enhanced active sites) from C-Mo bonds at the interface of MoS2 and HG.
These structure characteristics, electronic properties and moderate hydrogen adsorption energy contribute to the excellent HER performance achieved on the optimized MoS2/HG hybrid catalyst. A low overpotential of 124 mV at the current density of 10 mA cm−2 and a small Tafel slope of 41 mV dec−1 have been achieved together with long-term durability for 24 h continuous operation at 30 mA cm−2 and without observable fading. This strategy paves a way to design and develop other highly efficient, stable, and noble metal-free HER electrocatalysts.
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