Boosting the photocatalytic H2 evolution activity of type-II g-GaN/Sc2CO2 van der Waals heterostructure using applied biaxial strain and external electric field

Two-dimensional (2D) van der Waals (vdW) heterostructures are a new class of materials with highly tunable bandgap transition type, bandgap energy and band alignment. Herein, we have designed a novel 2D g-GaN/Sc2CO2 heterostructure as a potential solar-driven photocatalyst for the water splitting process and investigate its catalytic stability, interfacial interactions, and optical and electronic properties, as well as the effects of applying an electric field and biaxial strain using first-principles calculation. The calculated lattice mismatch and binding energy showed that g-GaN and Sc2CO2 are in contact and may form a stable vdW heterostructure. Ab initio molecular dynamics and phonon dispersion simulations show thermal and dynamic stability. g-GaN/Sc2CO2 has an indirect bandgap energy with appropriate type-II band alignment relative to the water redox potentials. Meanwhile, the interfacial charge transfer from g-GaN to Sc2CO2 can effectively separate electron-hole pairs. Moreover, a potential drop of 3.78 eV is observed across the interface, inducing a built-in electric field pointing from g-GaN to Sc2CO2. The heterostructure shows improved visible-light optical absorption compared to the isolated g-GaN and Sc2CO2 monolayers. Our study demonstrates that tunable electronic and structural properties can be realised in the g-GaN/Sc2CO2 heterostructure by varying the electric field and biaxial strain. In particular, the compressive strain and negative electric field are more effective for promoting hydrogen production performance. Since it is challenging to tune the electric field and biaxial strain experimentally, our research provides strategies to boost the performance of MXene-based heterojunction photocatalysts in solar harvesting and optoelectronic devices.