Two nanoribbon heterostructures are suitable for driving efficient direct Z-schemes of the photocatalytic overall water splitting for hydrogen production and are screened out of nine heterostructures constructed from edge-passivated antimonene (SbNR-X) and arsenide (AsNR-X, X = F, Cl, CN) nanoribbons. The solar-to-hydrogen (STH) efficiency and the Gibbs free energies (ΔGs) of the redox reactions at different sites are calculated to identify the preferable Z-schemes. Meanwhile, the transfer and recombination of the photogenerated carriers are explored by using nonadiabatic molecular dynamics (NAMD) simulations. The obtained band alignments and built-in electric fields of the two considered heterostructures can match the requirements of the photocatalytic Z-scheme, and the corresponding STH efficiencies can reach 15.04 % and 30.53 %, respectively. The oxidation evolution reactions can proceed spontaneously, and hydrogen evolution reactions are feasible in thermodynamics. NAMD simulations show that the SbNR-CN/AsNR-CN nanoribbon heterostructure has faster interlayer recombination but slower transfer of the photogenerated electron from the SbNR-CN to AsNR-CN nanoribbons and of the photogenerated hole along the reversible direction, indicating that this heterostructure has a higher carrier utilization rate. These findings confirm that the SbNR-CN/AsNR-CN nanoribbon heterostructure is a promising candidate for developing high STH efficiency materials with direct Z-schemes.
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