Ab Initio Quantum Dynamics Simulation of the Impact of Graphene on the Carrier Lifetime of the ZnV2O6 Photocatalyst.

ABSTRACT

We used a nonadiabatic molecular dynamics simulation to determine the carrier dynamics of a graphene/ZnV2O6 heterostructure in the search for an effective photocatalyst material. The C-2p orbital promotes the wave function overlap, guiding electrons to move between graphene and ZnV2O6, successfully achieving good mixing with the valence and conduction bands in ZnV2O6 materials, which is conducive to supporting carrier migration. The overlap between graphene/ZnV2O6 electrons and hole wave functions is less than that of ZnV2O6, and there is small absolute nonadiabatic coupling. The charge separation caused by graphene increases the carrier lifetime and prevents nonradiative electron-hole recombination. This study reveals the microscopic mechanism of extending the carrier lifetime of ZnV2O6 by introducing graphene, providing useful insights for regulating the electronic structure, promoting electron transfer and ultrafast electron and hole transfer. This strategy provides design considerations for advanced photocatalytic materials.