Insights into Photogenerated Carrier Dynamics and Overall Water Splitting of the CrS 3 /GeSe Heterostructure.

Based on the nonadiabatic molecular dynamics (NAMD) simulations and the first-principles calculations, we explore the overall water-splitting schemes and the photogenerated carrier dynamics for two configurations (CG and C y G) of the CrS 3 /GeSe van der Waals heterostructures. The photocatalytic direct Z-schemes and carrier migration pathways for hydrogen and oxygen evolution reactions (HER/OER) are constructed based on the electronic properties. The solar-to-hydrogen efficiency (η' STH values) of the schemes can reach 10.60% and 10.17% and further rise under tensile strain. The NAMD results demonstrate similar transfer times of the electron/hole for HER/OER and more rapid electron-hole recombination in CG enables it to be superior to C y G in photocatalytic performance. Moreover, the Gibbs free energy indicates that both the HERs and OERs turn to spontaneously proceed with CG and C y G at pH = 0-12.37 and pH = 2.55-11.01, respectively. These facts reveal that the CrS 3 /GeSe heterostructure is promising in photocatalytic overall water splitting.