Theoretical investigation on interactions between lithium ions and two-dimensional halide perovskite for solar-rechargeable batteries

Abstract

Two-dimensional (2D) halide perovskite materials have recently been proposed for solar energy conversion and energy storage systems, namely, photo-rechargeable batteries. However, the theoretical understanding of the 2D halide perovskite materials for the photo-rechargeable batteries lags behind the experimental advancement. In this manuscript, we investigate the adsorption and transport properties of lithium ions on an experimentally verified 2D halide perovskite material, (C6H9C2H4NH3)2PbI4, via first-principles calculations. Our study reveals the efficient adsorption and transport properties of the lithium ion at the 2D lead halide perovskite surface, and demonstrates the prospects of the metal halide perovskite system as an effective anode material for lithium-ion batteries as well as the photo-charging medium for photo-rechargeable batteries. In addition, the interlayer diffusion of the lithium ions is calculated, which demonstrates the efficient transport of the lithium ions between the 2D halide perovskite layers that contribute to the most of capacity. Most importantly, the displacement of the lithium ion is demonstrated to be available upon the hole polaron formation, which is suggested to signify the photo-charging behaviour initiating the unidirectional lithium ion movement on the electrode surface. The present study for the first time rationalizes the photo-charging behaviour of the photo-rechargeable battery, and facilitates the fundamental understanding on the halide perovskites for the energy storage applications including the lithium-ion batteries and the photo-rechargeable batteries.