Two-dimensional trilayer heterostructures with cascade dual Z-schemes to achieve efficient hydrogen evolution reaction

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2024-01, Vol.12 (4), p.2359-2372
• Main Authors: Wan, Xue-Qing, Yang, Chuan-Lu, Li, Xiao-Hu, Liu, Yu-Liang, Zhao, Wen-Kai
• Format: Article
• Language: English
• Subjects: First principles; Free energy; Gibbs free energy; Heterostructures; Hydrogen; Hydrogen evolution reactions; Hydrogen production; Molecular dynamics; Oxygen evolution reactions; Photocatalysis; Water splitting
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/d3ta06755f

Cascade dual Z-schemes for photocatalytic overall water splitting for hydrogen production are constructed for trilayer Bi/HfSeTe/ZrSe 2 , Bi/HfSeTe/ZrSe 2 , and InAs 3 /HfSeTe/ZrSe 2 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/ZrSe 2 and InAs 3 /HfSeTe/ZrSe 2 heterostructures are explored, and those for the HfSe 2 /ZrSe 2 /HfSe 2 and ZrSe 2 /HfSe 2 /ZrSe 2 sandwich heterostructures are also considered for comparison. The solar-to-hydrogen efficiency of 22.08% for the bilayer HfSeTe/ZrSe 2 heterostructure can be raised to 40.52%, 39.47%, and 41.04% by the cascade dual Z-schemes with Bi/HfSeTe/ZrSe 2 , Bi/HfSeTe/ZrSe 2 , and InAs 3 /HfSeTe/ZrSe 2 . 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/ZrSe 2 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. Electronic properties and diabatic molecular dynamics simulations reveal that the maximum solar-to-hydrogen efficiency of photocatalytic cascade dual Z-schemes with Bi(InAs 3 )/HfSeTe/ZrSe 2 heterostructures can reach 41.04%.