The stable operation of lithium (Li) metal anode heavily relies on the intrinsic surface chemistry. However, the correlations between the composition of solid-electrolyte interphase (SEI) and its impact on working Li anode are insufficiently understood, which significantly restrains the efficiency for directional interfacial design. In this contribution, the interfacial transfer kinetics of solvated Li ions (Li⁺) regarding three model SEIs which possess similar components but various inorganic contents was systematically investigated. A general correlation was demonstrated that inorganics-rich SEI contributes to a lower energy barrier for the interfacial journey of solvated Li⁺, which involves a facile de-solvation process and a rapid ion diffusion through SEI. Lower overpotentials for both initial Li nucleation and interfacial activation processes were identified with a three-electrode cell configuration ascribed to the reduced energy barrier at the interphase, which potentially facilitate a compact and dense Li plating feature. This work sheds light on the relations between SEI property and the interfacial transfer kinetics of solvated Li⁺, aiming to provide more fundamental insights into the interfacial manipulation for a low-resistance and stable working Li metal batteries.

锂（Li）金属阳极的稳定运行在很大程度上取决于本征表面化学性质。然而，人们对固态电解质界面相（SEI）的组成及其对工作锂阳极的影响之间的相关性了解不足，这极大地限制了定向界面设计的效率。在这一贡献中，系统地研究了溶剂化锂离子（Li ⁺）关于三种具有相似成分但各种无机含量的模型SEI的界面转移动力学。普遍的相关性表明，富含无机物的SEI有助于降低溶剂化Li ⁺的界面行程的能垒。，这涉及轻松的去溶剂化过程和通过SEI进行的快速离子扩散。最初的Li成核过程和界面活化过程都具有较低的超电势，这是由于三电极电池结构引起的，该三电极电池结构归因于界面相处的能垒降低，潜在地促进了紧凑而致密的Li镀层特征。这项工作阐明了SEI性能与溶剂化Li ⁺的界面转移动力学之间的关系，旨在为低电阻和稳定工作的Li金属电池的界面操作提供更多基础见解。