Engineering Phase Stability of Semimetallic MoS₂Monolayers for Sustainable Electrocatalytic Hydrogen Production

1T′-phase MoS₂possesses excellent electrocatalytic performance, but due to the instability of the thermodynamic metastable phase, its actual electrocatalytic effect is seriously limited. Here, we report a wet-chemical synthesis strategy for constructing rGO/1T′-MoS₂/CeO₂heterostructures to improve the phase stability of metastable 1T′ phase MoS₂monolayers. Importantly, the rGO/1T′-MoS₂/CeO₂heterostructure exhibits excellent electrocatalytic hydrogen evolution reaction (HER) performance, which is much better than the 1T′-MoS₂monolayers. The synergistic effects between CeO₂nanoparticles (NPs) and 1T′-MoS₂monolayers were systematically investigated. 1T′-MoS₂monolayers combined with the cocatalyst of CeO₂NPs can produce lattice strain and distortion on 1T′-MoS₂monolayers, which can tune the energy band structure, charge transfer, and energy barriers of hydrogen atom adsorption (ΔE_H), leading to promotion of the phase activity and stability of 1T′-MoS₂monolayers for hydrogen production. Our work offers a feasible method for the preparation of efficient HER electrocatalysts based on the engineering phase stability of metastable materials.