发表机构
Seoul National University（首尔大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过压力感知机器学习分子动力学方法，揭示了压力大小、加载几何对锂金属-硫化物电解质界面中间相形成的非单调调控作用，为硫化物固态电池压力效应提供了机制框架。
AI 中文摘要
叠片压力通常被视为全固态锂金属电池中维持物理接触的手段，但它也能改变反应性固-固界面的化学性质。本研究采用经密度泛函理论（DFT）验证的压力感知、电荷分辨机器学习分子动力学方法，探究压力大小和加载几何对Li||Li6PS5Cl界面中间相形成的调控作用。该响应呈非单调特性：1千巴（kbar）的压缩会加速PS4分解及类Li2S有序化，而10至100千巴的压缩则会限制结构重排与长程结晶。电荷分辨动力学进一步识别出与后续类Li2S有序化相关的富锂硫中心早期中间相环境。在相同标称压力下，单轴加载比等静压加载更能加速界面反应。压力还会以缺陷位置依赖的方式改变孔隙闭合与死锂扩散。这些结果确立了外加压力为耦合中间相化学、离子传输与缺陷演化的机械化学过程变量，为解释硫化物固态电池中的压力效应提供了机制框架。
英文摘要
Stack pressure is commonly treated as a means of maintaining physical contact in all-solid-state lithium-metal batteries, but it can also alter the chemistry of reactive solid-solid interfaces. Here, using pressure-aware, charge-resolved machine-learning molecular dynamics validated against DFT, we determine how pressure magnitude and loading geometry regulate interphase formation at Li||Li6PS5Cl interfaces. The response is nonmonotonic: compression at 1 kbar accelerates PS4 decomposition and Li2S-like ordering, whereas 10-100 kbar compression restricts structural rearrangement and long-range crystallization. Charge-resolved dynamics further identify sulfur-centered, lithium-rich early-interphase environments associated with subsequent Li2S-like ordering. Uniaxial loading accelerates interfacial reaction relative to isostatic loading at the same nominal pressure. Pressure also changes void closure and dead-lithium spreading in a defect-location-dependent manner. These results establish applied pressure as a mechanochemical process variable coupling interphase chemistry, ion transport and defect evolution, providing a mechanistic framework for interpreting pressure effects in sulfide solid-state batteries.
