Two-dimensional trilayer heterostructures with cascade dual Z-schemes to achieve efficient hydrogen evolution reaction†
Abstract
Cascade dual Z-schemes for photocatalytic overall water splitting for hydrogen production are constructed for trilayer Bi/HfSeTe/ZrSe2, Bi/HfSeTe/ZrSe2, and InAs3/HfSeTe/ZrSe2 heterostructures. Electronic properties are studied by first-principles calculations, and the photoexcited carrier pathway is explored by nonadiabatic molecular dynamics simulations. The arrow-up, arrow-down, and cascade arrangement of band alignments for the Bi/HfSeTe/ZrSe2 and InAs3/HfSeTe/ZrSe2 heterostructures are explored, and those for the HfSe2/ZrSe2/HfSe2 and ZrSe2/HfSe2/ZrSe2 sandwich heterostructures are also considered for comparison. The solar-to-hydrogen efficiency of 22.08% for the bilayer HfSeTe/ZrSe2 heterostructure can be raised to 40.52%, 39.47%, and 41.04% by the cascade dual Z-schemes with Bi/HfSeTe/ZrSe2, Bi/HfSeTe/ZrSe2, and InAs3/HfSeTe/ZrSe2. They can further be boosted to 41.53%, 41.12%, and 43.57% under 1%, 1%, and −2% biaxial strains, respectively. The nonadiabatic molecular dynamics simulations reveal that the activity of the photogenerated carriers can be well protected. Moreover, the Gibbs free energy changes demonstrated that the hydrogen and oxygen evolution reactions driven by Bi/HfSeTe/ZrSe2 can spontaneously proceed. Therefore, the cascade dual Z-scheme provides an effective way to develop highly efficient photocatalysts for hydrogen generation from overall water splitting.
- This article is part of the themed collection: Today's Simulations: Pioneering the Experiments of Tomorrow