Abstract
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/Sc(2)CO(2) 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 Sc(2)CO(2) 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/Sc(2)CO(2) 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 Sc(2)CO(2) 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 Sc(2)CO(2). The heterostructure shows improved visible-light optical absorption compared to the isolated g-GaN and Sc(2)CO(2) monolayers. Our study demonstrates that tunable electronic and structural properties can be realised in the g-GaN/Sc(2)CO(2) 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.