鋰硫電池因具有高理論能量密度（2600 Wh kg⁻¹）、低成本與環境友善等優勢，被視為具潛力的次世代儲能系統。然而，鋰硫電池在實際應用上仍受到多硫化物穿梭效應、活性物質流失、介面副反應與循環壽命不足等問題限制。除了硫陰極端的反應不穩定外，鋰金屬陽極介面的劣化亦是影響鋰硫電池長循環性能的重要因素。在反覆鋰沉積/剝離過程中，鋰金屬表面之固態電解質介面層（solid electrolyte interface, SEI）容易破裂與再生成，使新鮮鋰金屬持續暴露於電解液與多硫化物環境中，進而造成副反應、非活性鋰累積、介面阻抗上升與容量衰退。此外，傳統研究常使用過量鋰箔作為陽極，雖可延長循環時間，但過量鋰源可能掩蓋介面副反應與鋰耗損，使電池壽命被高估，進而不利於評估保護層在有限鋰源條件下的實際保護效果。因此，若要提升鋰硫電池的實際能量密度與長循環穩定性，必須在薄鋰陽極條件下建立穩定且具鋰離子傳輸能力的保護介面。本研究以 Li₃PS₄（LPS）作為鋰金屬表面保護層，並將 20 wt% LPS 漿料塗佈於不同厚度鋰箔表面，形成厚度約 80 μm 的 LPS 保護層。此保護層具有鋰離子傳輸能力與電子阻隔特性，可降低鋰金屬與電解液以及多硫化物的直接接觸，並改善鋰離子於介面上的傳輸均勻性。為系統性評估 LPS 保護層之介面保護效果，本研究分別以鋰//鋰對稱電池、鋰//銅半電池與鋰硫電池進行驗證，探討其對鋰沉積/剝離穩定性、鋰利用可逆性與鋰硫電池循環壽命之影響。在鋰//鋰對稱電池中，LPS 保護層可於電流密度 1 mA cm-2與面積容量 1 mAh cm-2 的條件下，使鋰厚度為 300 μm 與 50 μm 的電池皆能穩定循環達 1500小時與750小時。在鋰//銅半電池中，使鋰厚度為 300 μm 與 50 μm 的電池，皆能達到 140 週與 80 週，同時庫倫效率穩定維持在約 96%。進一步應用於鋰硫電池時，LPS 保護層鋰金屬在不同鋰厚度下皆展現較穩定的循環表現：在 C/10 倍率下可穩定運行約500 週，而在 C/5、C/2 以及 1 C 倍率下也能維持 1000週的長循環穩定性。本研究結果顯示，LPS 保護層可在鋰金屬表面建立穩定且具鋰離子傳輸能力的保護介面，使鋰沉積/剝離行為更加均勻，並降低非活性鋰與介面副反應產物的累積。相較於未修飾鋰金屬，LPS 保護層在鋰//鋰對稱電池、鋰//銅半電池與鋰硫電池中皆展現較佳的介面穩定性與循環表現，且在 50 μm 薄鋰條件下仍能維持穩定運作。此結果說明，LPS 保護層不僅可改善鋰金屬陽極的介面反應，也有助於推動薄鋰陽極於高能量密度鋰硫電池中的應用。

In this study, a Li₃PS₄ (LPS) artificial interface was coated on lithium metal foil to improve the stability of lithium-metal anodes. The LPS layer was introduced to regulate the interfacial reaction between lithium metal and the electrolyte, promote uniform Li ion transport, and reduce unstable lithium deposition during repeated cycling. Since direct contact between freshly deposited lithium and the electrolyte can continuously consume active lithium and electrolyte, the LPS coating serves as a protective barrier that helps stabilize the stripping/plating process. In addition, the favorable ionic conductivity of LPS and its compatibility with lithium metal contribute to a more stable interface, thereby suppressing dendrite growth and decreasing the formation of inactive lithium. The electrochemical performance of LPS-coated lithium was examined using symmetric Li/Li cells, Li/Cu half-cells, and Li–S batteries. In symmetric Li/Li cells, the LPS coating maintains a low overpotential and enables stable cycling up to 1500 hours and 750 hours for lithium thickness of 300 μm and 50 μm, respectively, under a current density of 1 mA cm⁻² and an areal capacity of 1 mAh cm⁻². In Li/Cu half-cells, the LPS-coated lithium foils with thicknesses of 300 μm and 50 μm sustain stable cycling for up to 140 cycles and 80 cycles, respectively, while maintaining a Coulombic efficiency of approximately 96%. In Li–S batteries, both 300 μm and 50 μm LPS coating demonstrate stable cycling. The cell operates consistently for about 500 cycles at C/10 rate while at higher rates of C/5, C/2, and 1 C, it maintains performance for 1000 cycles. These results indicate that the LPS coating effectively stabilizes the lithium-metal interface across a range of cell configurations and lithium thickness conditions. The improved interfacial stability enhances the reversibility of lithium stripping/plating, reduces the generation of inactive lithium, and supports long-term cycling under both low- and high-rate conditions. Overall, this study demonstrates the potential of LPS coating as a practical anode modification strategy for high-energy-density Li–S batteries. It also provides a useful reference for future interface design in solid-state electrolytes and other advanced rechargeable battery systems.

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