Abstract
A novel sheet-on-sheet architecture with abundant sulfur vacancies (Vs) is designed by in situ growth of flake-like ZnIn(2)S(4) on the reduced graphene oxide (Vs-ZIS@RGO) surface, which serves as a functional layer on the separators for high-performance lithium-sulfur batteries (LSBs). Benefiting from the sheet-on-sheet architecture, the separators exhibit rapid ionic/electronic transfer, which is capable of supporting fast redox reactions. The vertically ordered ZnIn(2)S(4) shortens the diffusion pathways of lithium-ions and the irregularly curved nanosheets expose more active sites to effectively anchor lithium polysulfides (LiPSs). More importantly, the introduction of Vs adjusts the surface or interface electronic structure of ZnIn(2)S(4), enhancing the chemical affinity to LiPSs while accelerating conversion reaction kinetics of LiPSs. As expected, the batteries with Vs-ZIS@RGO modified separators exhibit an initial discharge capacity of 1067 mA h g(-1) at 0.5C. Even at 1C, the excellent long cycle stability (710 mA h g(-1) over 500 cycles) with an ultra-low decay rate of 0.055% per cycle is also attained. This work proposes a strategy of designing the sheet-on-sheet structure with rich sulfur vacancies, which provides a new perspective to rationally devise durable and efficient LSBs.