Interfacial Electronic States of GeC/g‐C3N4 van der Waal Heterostructure with Promising Photocatalytic Activity via Hydrogenation

Abstract

AbstractThe bandgap of most known two‐dimensional materials can be tuned by hydrogenation, although certain 2D materials lack a sufficient wide bandgap. Currently, it would be perfect to design non‐toxic, low‐cost, and high‐performance photocatalysts for photocatalytic water splitting via hydrogenation. We systematically examine the impact of hydrogenation on the optical and electronic characteristics of GeC/g‐C3N4 vdW heterostructures (vdWHs) with four different stacking patterns using first‐principles calculations. The phonon spectra, interlayer distance, binding energies and ab initio molecular dynamics calculations show the kinetic, mechanical, and thermal stability of GeC/g‐C3N4 vdWH after hydrogenation at 300, 500 and 800 K and possesses anisotropic Poisson's ratio, Young's and bulk modulus, suggesting that it's a promising candidate for experimental fabrication. According to an investigation of its electronic properties, GeC/g‐C3N4 vdWH has a bandgap of 1.28 eV, but hydrogenation dramatically increases it to 2.47 eV. As a result of interface‐induced electronic doping, the electronic states in g‐C3N4 might be significantly adjusted by coming into contact with hydrogenated GeC sheets. The vdWH exhibits a type‐II semiconductor, which can enhance the spatial separation of electron‐hole pairs and has a strong red‐shift of absorption coefficient than those of the constituent monolayers. The high potential drop caused by the significant valence and conduction band offsets effectively separated the charge carriers. The absorption coefficient of GeCH2/g‐C3N4 vdWH is highly influenced by a biaxial compressive strain more than the biaxial tensile strain. Our theoretical research implies that the hydrogenated GeCH2/g‐C3N4 vdWH possesses tunable optical and electronic behaviour for use as a hole‐transport material in solar energy harvesting, nanoelectronic and optoelectronic devices.