本研究採用Li0.33La0.557TiO3(LLTO)奈米線複合PVDF-HFP (Poly(vinylidene fluoride-co-hexafluoropropylene)製備陶瓷複合電解質，以此來降低聚合物基體的結晶度，提升Li離子遷移率。LLTO奈米線可以形成連續的通道，能提供鋰離子連續性的傳遞，離子導率提升至1.50 x 10-4S cm-1。為了改善PVDF-HFP與Li界面的副反應，本研究提出少量LITFSI/FEC/SN離子導體修飾界面，以此提升LiF在固態電解質介面層(SEI)的比例，透過提升LiF含量來完全抑制PVDF-HFP與Li的副反應。在長時間恆電流循環充放電過程，電壓維持穩定並且持續560小時後，沒有發現副反應的跡象，與傳統液態電解質修飾界面相比提升約41 %穩定性。在恆電流循環後，從SEM表面影像顯示當CPE有副反應時，在Li表面有大量鋰樹枝晶與死鋰生成，而CPE沒有副反應時，Li表面平整且均勻。透過XPS分析CPE與Li表面元素分析證明SNE修飾CPE與Li之界面可以完全抑制副反應。此外，LFP|SNE|CPE|SNE|Li全電池在0.2 C下循環100圈後，比電容量仍保持在134 mAh g-1，庫侖效率為仍保持在98.5%，幾乎沒有容量損失（5 th：135.4 mAh g-1 和 100 th：134 mAh g-1）。這項研究顯示離子導體和兼容的界面，對 ASSLMB(All-solid-state lithium-metal battery)至關重要，特別是對於界面處的穩定性。;In this study, Li0.33La0.557TiO3(LLTO) nanowires were used as ceramic fillers in PVDF-HFP-based electrolytes to reduce the crystallinity of the polymer matrix. The LLTO nanofibers also provide continuous channels that facilitate Li+ transport. The ionic conductivity were increased to 1.50*10-4 S-cm-1, about 10 times higher than that of the pure PVDF-HFP electrolyte without LLTO. We further proposed a composite polymer electrolyte using plastic superionic conductor succinonitrile-based electrolyte (LITFSI/FEC/SN, SNE), where little amounts of succinonitrile-based conductor were applied at the interface between Li electrode and PVDF-HFP-based composite polymer electrolyte. The addition of FEC to SNE increased the ratio of lithium fluoride (LiF) in the solid electrolyte interface (SEI) and inhibited the side reaction of PVDF-HFP. In the long-term galvanostatic cycle charge-discharge testing, the voltage remained stable for 560 hours and the stability improved about 41% compared to LE-modified CPE. The XPS analysis indicated that the side reactions were completed inhibited after SNE modification of CPE. Moreover, the LFP|SNE|CPE|SNE|Li cell has a discharge specific capacity of 134 mAh g−1 at 0.2 C after 100 cycles and a Coulombic efficiency of 98.5% without virtually capacity loss (135.4 mAh g−1 after 5 cycles and 134 mAh g−1 after 100 cycles). This work demonstrated that the super-conductive electrolyte and compatible interface are both crucial for improving ionic conductivity and SEI stability in a high performance ASSLMB.
