High carrier mobility ZrSSe/SnX (X=S, Se, S₂, Se₂) vdW heterostructures for photocatalytic overall water splitting: A first-principles study

Recently, the assembly of novel two-dimensional materials via van der Waals (vdW) interactions to form heterostructures is considered an effective strategy for producing materials with enhanced photocatalytic activities. This study systematically explored the optoelectronic and photocatalytic properties and carrier mobilities of novel ZrSSe/SnX (X = S, Se, S2, Se2) vdW heterostructures using density functional theory. The formation energies, elastic constants, phonon dispersions, and results of ab-initio molecular dynamic simulations indicate structural, mechanical, dynamic, and thermal stability. The electronic band structure and optical properties are calculated using hybrid functional HSE06 for accurate calculations. The results of calculations using the bandgap center technique based on density functional theory show that ZrSSe/SnSe, ZrSSe/SnS2, and ZrSSe/SnSe2 heterostructures possess suitable band edges for photocatalytic overall water splitting. The optical absorption spectrum covers a broad range from 104 in the visible region and increases to 105 in the UV region. Furthermore, the ZrSSe/SnX (X = S, Se, S2, Se2) heterostructures have high carrier mobilities of the order of 105. High mobilities help carriers to move quickly and reduce the recombination rate of holes and electrons. The findings indicate that ZrSSe/SnX (X = S, Se, S2, Se2) heterostructures are potentially efficient visible-light photocatalysts for overall water splitting.