The interface between lithium metal and solid electrolytes (SEs) has a significant impact on the performance of lithium-metal batteries, especially when the electrolyte is unstable and decomposes into different components, leading to structural and morphological changes. However, current knowledge of the interface upon decomposition, such as the Li/LiPON interface, is limited, particularly at the atomic level. Here, we use first-principles calculations to elucidate the interfacial stability and structural properties of possible interfaces formed between the lithium-metal electrode and the decomposition products of LiPON. Through a systematic study and comparison of these interfaces, we have identified an interfacial stability sequence of Li/Li₂O > Li/Li₃N > Li/Li₃P > Li/Li₃PO₄, suggesting that the lithium-metal anode will predominantly form an interface with Li₂O after the decomposition of LiPON. Moreover, the low interfacial energy and high work of adhesion of Li/Li₂O suggest that the formation of a Li/Li₂O interface in LiPON may promote interfacial stability and potentially inhibit the defect and dendrite formation at the interface. This provides an explanation for the known compatibility of LiPON with lithium-metal anodes. Our findings reveal the critical role of the Li/Li₂O interface formation after the decomposition of LiPON at the Li/LiPON interface, which encourages further investigation and design of the lithium-metal anode/SE interface in all solid-state batteries.

中文翻译：

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从分子水平洞察Li/LiPON界面：界面分解与重构


锂金属和固体电解质（SE）之间的界面对锂金属电池的性能有显着影响，特别是当电解质不稳定并分解成不同的成分，导致结构和形态变化时。然而，目前对分解界面（例如 Li/LiPON 界面）的了解是有限的，特别是在原子水平上。在这里，我们使用第一性原理计算来阐明锂金属电极和 LiPON 分解产物之间可能形成的界面的界面稳定性和结构特性。通过对这些界面的系统研究和比较，我们确定了界面稳定性顺序为Li/Li ₂ O > Li/Li ₃ N > Li/Li ₃ PO ₄ ，表明 LiPON 分解后，锂金属阳极将主要与 Li ₂ O 形成界面。此外，Li/Li ₂ O 的低界面能和高粘附功表明 LiPON 中 Li/Li ₂ O 界面的形成可能会促进界面稳定性并可能抑制界面处的缺陷和枝晶形成。这为 LiPON 与锂金属阳极的已知兼容性提供了解释。我们的研究结果揭示了 LiPON 在 Li/LiPON 界面分解后 Li/Li ₂ O 界面形成的关键作用，这鼓励了对锂金属负极/SE 界面的进一步研究和设计。固态电池。