Theoretical prediction of the electronic structure, optical properties and photocatalytic performance of type-I SiS/GeC and type-II SiS/ZnO heterostructures

Nowadays, it would be ideal to develop high-performance photovoltaic devices as well as highly efficient photocatalysts for the production of hydrogen via photocatalytic water splitting, which is a feasible and sustainable energy source for addressing the challenges related to environmental pollution and a shortage of energy. In this work, we employ first-principles calculations to investigate the electronic structure, optical properties and photocatalytic performance of novel SiS/GeC and SiS/ZnO heterostructures. Our results indicate that both the SiS/GeC and SiS/ZnO heterostructures are structurally and thermodynamically stable at room temperature, suggesting that they are promising materials for experimental implementation. The formation of SiS/GeC and SiS/ZnO heterostructures gives rise to reduction of the band gaps as compared to the constituent monolayers, enhancing the optical absorption. Furthermore, the SiS/GeC heterostructure possesses a type-I straddling gap with a direct band gap, while the SiS/ZnO heterostructure forms a type-II band alignment with indirect band gap. Moreover, a red-shift (blue-shift) has been observed in SiS/GeC (SiS/ZnO) heterostructures as compared with the constituent monolayers, enhancing the efficient separation of photogenerated electron-hole pairs, thereby making them promising candidates for optoelectronic applications and solar energy conversion. More interestingly, significant charge transfers at the interfaces of SiS-ZnO heterostructures, have improved the adsorption of H, and the Gibbs free energy ΔH* becomes close to zero, which is optimal for the hydrogen evolution reaction to produce hydrogen. The findings pave the path for the practical realization of these heterostructures for potential applications in photovoltaics and photocatalysis of water splitting. © 2023 The Royal Society of Chemistry.