Simultaneous Manipulation of O-Doping and Metal Vacancy in Atomically Thin Zn10 In16 S34 Nanosheet Arrays toward Improved Photoelectrochemical Performance.

The facile hydrothermal synthesis of Zn10 In16 S34 atomically thin nanosheet arrays on fluorine-doped tin oxide glass (FTO) substrates is presented. Through controlling heat treatment in air, O-doping and Zn, S vacancies were simultaneously introduced in Zn10 In16 S34 nanosheets with adjusted phase, morphology, chemical compositions, and energy level distribution. The surface defect states are passivated by depositing ultrathin Al2 O3 film by atomic layer deposition technology. The performance of Zn10 In16 S34 photoanodes is largely improved, with 4.7 times higher current density and reduced onset potential. The experimental results and density functional theory calculations indicate that the enhancement is attributed to the fast photoexcited electron-hole pair separation, decreased surface transfer impedance, prolonged carrier lifetime, and reduced overpotential of oxygen evolution reaction.