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.

中文翻译：

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太阳能充电电池锂离子与二维卤化物钙钛矿相互作用的理论研究

摘要 二维（2D）卤化物钙钛矿材料最近被提出用于太阳能转换和储能系统，即光充电电池。然而，对用于光充电电池的二维卤化物钙钛矿材料的理论理解落后于实验进展。在本手稿中，我们通过第一性原理计算研究了锂离子在经过实验验证的二维卤化物钙钛矿材料 (C6H9C2H4NH3)2PbI4 上的吸附和传输特性。我们的研究揭示了锂离子在二维卤化铅钙钛矿表面的高效吸附和传输特性，并展示了金属卤化物钙钛矿体系作为锂离子电池有效负极材料以及光充电电池的光充电介质的前景。此外，计算了锂离子的层间扩散，这证明了锂离子在有助于最大容量的二维卤化物钙钛矿层之间的有效传输。最重要的是，锂离子的位移被证明在空穴极化子形成时是可用的，这表明光充电行为引发了电极表面上的单向锂离子运动。本研究首次合理化了光充电电池的光充电行为，