Strain Engineering the Optoelectronic and HER Behavior of MoS2/ZnO Heterojunction: A DFT Investigation

The rational design of heterojunctions by coupling two or more two-dimensional (2D) materials is regarded as a feasible strategy to efficiently enhance photocatalytic-hydrogen performance by capturing solar energy to address the increasing global energy crisis. In this work, a functional MoS₂/ZnO heterojunction is proposed based on first-principles simulation. Our results reveal that the photogenerated electrons and holes in the MoS₂/ZnO heterojunction follow a specific Z-scheme pathway, highly facilitating redox reactions and optimizing optical properties in the visible-light region. Under external strain, the MoS₂/ZnO heterojunction demonstrates improved HER performance and remarkable optical-harvesting capabilities. Interestingly, the HER free energy for the heterojunction is only −0.04 eV under −5% compressive strain, highlighting its promising potential for photocatalytic hydrogen production. We observe that the absorption edge of the spectrum shifts gradually to the infrared region with increasing tensile biaxial strains, whereas compressive biaxial strains result in a blue-shift absorption spectrum. Additionally, all heterojunctions achieve excellent solar-to-hydrogen (STH) efficiencies exceeding 10%, demonstrating their capability to store sufficient solar energy. Our work offers a novel strategy for exploring highly efficient photocatalysts in the field of hydrogen energy with the ability to modulate their activity through external strain.