本研究旨在提升鋰金屬電池的安全性與鋰離子傳輸效率，提出以聚磷酸鋰（lithium polyphosphate, LPP）包覆二氧化矽（SiO₂）粒子所構成之複合功能性塗層材料（SiO₂@LPP），應用於隔離膜表面。LPP具偏負電性，可選擇吸引鋰離子並具備阻燃性；SiO₂則提供機械支撐與熱穩定性。由物理吸附製備之SiO₂@LPP塗層能結合上述特性，期能強化電池整體安全性與電化學性能。
材料特性方面，透過SEM、EDS、DLS與XPS確認LPP均勻包覆SiO₂顆粒之形貌與元素分布，接觸角測試亦驗證塗層可提升對極性電解液之潤濕性。在高溫安全性方面，SiO₂@LPP塗層可減緩隔離膜形變，且LPP於高溫下裂解可捕捉氫自由基，縮短燃燒時間與抑制火焰蔓延；SiO₂則作為高機械強度之不可燃隔離塗層降低高溫下隔離膜形變量，並減少氧氣與電解液於燃燒過程中的接觸，進一步避免燃燒。
電化學性能方面，塗層提升濕潤性使離子導電度上升。拉曼分析顯示，LPP偏負電荷可與溶劑爭搶鋰離子，始界面鋰離子濃度上升而加速鋰離子擴散，促進均勻沉積並抑制枝晶生成。靜置阻抗與循環測試亦顯示，負電表面可能藉由排斥陰離子，降低鈍化層生成，維持較低的電荷轉移阻抗並增進界面穩定性。此外，交換電流密度與鋰對稱電池測試結果顯示，在高電流密度下，SiO₂@LPP可承受更高電流密度的沉積剝離並擁有較高界面反應效率。
綜上，SiO₂@LPP複合塗層兼具機械強度、阻燃性與鋰離子選擇性引導能力，可有效改善高溫形變、抑制燃燒、提升界面穩定性與充放電效率，展現鋰金屬電池系統於高安全性與高效能應用的潛力，為未來高電流密度儲能系統提供材料設計依據。

This study aims to enhance the safety and lithium-ion transport efficiency of lithium metal batteries by proposing a composite functional coating material (SiO₂@LPP), consisting of lithium polyphosphate (LPP) coated on silicon dioxide (SiO₂) particles, applied to the surface of battery separators. LPP carries partial negative charges, allowing for selective attraction of lithium ions and exhibiting excellent flame-retardant properties, while SiO₂ provides mechanical support and thermal stability. The physically adsorbed SiO₂@LPP coating integrates these features to improve overall battery safety and electrochemical performance.
In terms of material characterization, SEM, EDS, DLS, and XPS analyses confirm the uniform coating morphology and elemental distribution of LPP on SiO₂ particles. Contact angle measurements further verify that the coating enhances wettability toward polar electrolytes. Regarding thermal safety, the SiO₂@LPP coating mitigates separator deformation under high temperatures. LPP decomposes at elevated temperatures to capture hydrogen radicals, thereby shortening combustion duration and suppressing flame propagation. Meanwhile, the high mechanical strength and nonflammable nature of SiO₂ helps reduce separator deformation and minimizes contact between oxygen and electrolyte during combustion, further preventing ignition.
Electrochemically, improved wettability from the coating increases ionic conductivity. Raman spectroscopy reveals that the negatively charged LPP competes with solvents for lithium-ion coordination, enriching Li⁺ concentration at the interface and accelerating Li⁺ diffusion. This promotes uniform deposition and suppresses dendrite formation. Static impedance and cycling tests indicate that the negatively charged surface may repel anions, reduce passivation layer formation, maintain low charge transfer resistance, and enhance interfacial stability. Additionally, results from exchange current density calculations and lithium symmetric cell testing show that SiO₂@LPP enables more efficient interfacial reactions and supports stable stripping/plating behavior even at high current densities.
In summary, the SiO₂@LPP composite coating provides mechanical strength, flame retardancy, and lithium-ion selectivity, effectively addressing separator deformation, combustion, interfacial instability, and inefficient charge/discharge at high currents. This demonstrates its potential for safe and high-performance lithium metal battery systems and offers a valuable material design strategy for future high-current-density energy storage applications.

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