Single-layer GaInS3: Water-splitting photocatalyst with high solar conversion efficiency and long carrier lifetime from first-principles investigation

Two-dimensional (2D) materials with a high solar to hydrogen (STH) conversion are in high demand due to the escalating energy crisis and environmental degradation. The STH efficiency is strongly correlated with the charge carrier separation, which can be improved by the inside electric dipole. Herein, the water-splitting capabilities of single-layer (SL) GaInS3 are explored by employing first-principles calculations. Theoretical outcomes reveal that SL GaInS3 exhibits a large intrinsic electric dipole and has a thermally stable structure at 300 K. SL GaInS3 displays a direct bandgap of 1.83 eV, as well as suitable band edges and abundant visible absorption (105 cm−1) for solar-driven water-splitting. The electronic structure and carrier mobility calculations demonstrate the high separation efficiency of charge carriers, which is strongly affirmed by the quite long carrier lifetime of 8.26 ns. The overpotential analysis of charge carriers suggests that the oxygen generation of SL GaInS3 can be accomplished without a cocatalyst, while hydrogen generation can be completed with the aid of cocatalysts. The STH efficiency of SL GaInS3 reaches up to 16.8%, apparently surpassing the commercial standard (10%). In brief, the high STH and long carrier lifetime promise the possible application of SL GaInS3 for solar water splitting. What's more, this work provides straight evidence that 2D photocatalysts with inside dipoles exhibit a long carrier lifetime.