Abstract The solid electrolyte interface (SEI) not only play the role of surface protective film for lithium metal anodes in lithium-sulfur batteries but also use to suppress the growth of lithium dendrites during the charging process. The relationship between the morphology of the SEI and the deposition behavior of lithium atoms determines the effect of homogenization of the dendrites. The Li-halide (LiF, LiCl, and LiBr) solid electrolyte interface is comparatively investigates by comprehensive first-principles calculations on Li metal anodes. Surface adsorption, surface diffusion, and charge transfer of Li atoms during the deposition process on the Li-halide SEIs with aggregated Li–Ha2Li2 island configurations is systematically calculates to achieve the orientation of Li atoms from deposition. However, the Li atom has high migration energy regardless of the uniformity of the surface of LiF-SEI, which has high stability making the charge transfer of Li atoms less affected by the subneighbor and subsurface Ha atoms. The Li atom deposition behavior makes the charge transfer and lithium halide (LiHa) SEI potential tend to be evenly distributed, which in turn leads to uniform deposition of Li atoms.

中文翻译：

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SEI的卤化锂（F，Br，Cl）表面岛周围嵌入的锂原子的电荷转移：第一性原理计算

摘要 固体电解质界面（SEI）不仅在锂硫电池中起到了锂金属负极表面保护膜的作用，而且在充电过程中还起到抑制锂枝晶生长的作用。SEI 的形态与锂原子的沉积行为之间的关系决定了枝晶均匀化的效果。通过对锂金属负极的综合第一性原理计算，对卤化锂（LiF、LiCl 和 LiBr）固体电解质界面进行了比较研究。在具有聚集的 Li-Ha2Li2 岛构型的锂卤化物 SEI 上的沉积过程中，锂原子的表面吸附、表面扩散和电荷转移被系统地计算，以实现沉积中锂原子的取向。然而，无论 LiF-SEI 表面的均匀性如何，Li 原子都具有高迁移能，具有高稳定性，使得 Li 原子的电荷转移受亚邻域和亚表面 Ha 原子的影响较小。Li原子的沉积行为使电荷转移和卤化锂（LiHa）SEI电位趋于均匀分布，进而导致Li原子的均匀沉积。