固態電池普遍存在充放電壽命顯著低於鋰離子電池的問題，我們提出一種新穎的複合電解質，根據此電解質的固態鋰金屬電池，若充放電流0.1C，放電深度100%，圈數壽命(仍保有最高電容量的80%)可望達到575圈，且電容量接近理論值，若電流提高至0.2C – 0.5C，壽命與電容量都低於0.1C的表現，但仍有相當低的電容量充放損失及可觀的電容量。
複合電解質包括自製的氨酯-丙烯酸丁酯寡聚物(PUA)，聚偏二氟乙烯－共－三氯乙烯(PVdF-HFP)長鏈高分子，雙氟磺酼亞胺鋰(LiFSI)，石榴石結構鋰鑭鋯鉭氧(LLZTO)粉末，寡聚物乃是電解質的核心，聚合分子量6000 - 7000 g mol1，添加鋰鹽後玻璃轉化溫度低於室溫，21.1 C，因此混合PVdF-HFP後具有黏著劑的特性及充分的機械強度，研究中我們合成兩種複合電解質，自撐形式的膜電解質標示作PUA-FS，另一種電極塗層的電解質標示作PUA-EC。
PUA-FS及PUA-EC固態電解質的鋰離子遷移數與電位窗口很相似，鋰離子遷移數0.31-0.34，電位窗口為4.6 V，兩者均具有類似三明治的結構，離子導體PUA顆粒聚集成導管並包裹在富PVdF-HFP的表面膜中，兩者的組成不盡相同，PUA-FS需要更高含量的PVdF-HFP才能有充分的機械強度，因此PUA-FS的PUA含量低於PUA-EC，PUA-FS的導電性不如PUA-EC。在30°C時PUA-FS導電率為4.91×10-4 S cm-1，而PUA-EC則為5.7×10-4 S cm-1。
固態鋰離子電池的組合包括，陰極磷酸鋰鐵LFP，陽極鋰金屬，固態複合電解質PUA-FS或PUA-EC，充放電池窗口2.0 - 4.0 V，並在室溫下，以0.1C、0.2C、0.3C與0.5C進行恆電流充放電測試，充放電深度100%，PUA-FS電池在循環穩定性和C-rate容量方面明顯優於PUA-EC電池，PUA-FS電池0.1C放電電容量最高169.7 mAh g1，單圈電容量損失0.036%，而0.3C放電電容量最高為147.0 mAh g1，單圈電容量損失0.069%，目前0.1C充放電超過250個循環；0.3C充放電超過600個循環。

A common problem with solid-state battery is its cycle life is much shorter than those of lithium ion batteries. We prepare a novel composite electrolyte, and based on this electrolyte, the solid-state lithium metal battery displays a low capacity loss, an expected 575 cycles at 0.1C and 100% depth of discharge before its capacity drops to 80% of its maximum capacity. When the charging current is raised to 0.2C – 0.5C, the cycle life and capacity are less than those of 0.1C. Nonetheless, the performances as a solid-state battery are still respectable.
The composite electrolyte contains an in-house oligomer of polyurethane-acrylate-thiocarbonate (PUA), long-chain PVdF-HFP, LiFSI lithium salt, and LLZTO additive. The PUA oligomer is the core of composite electrolyte, 6000 - 7000 g mol1 in molecular weight. Its glass transition temperature is low with 30 wt% LiFSI, 21.1 C. Therefore, its PVdF-HFP mixture exhibits the properties of adhesive and sufficient mechanical strength. In this study, we synthesize two composite electrolytes; the free-standing membrane electrolyte denoted as PUA-FS, and the electrode-coated membrane electrolyte denoted as PUA-EC.
The two composite electrolytes share high similarities in lithium transference number (tLi+) and potential window (U); tLi+=0.31-0.34, U =4.6 V. Both have a sandwich-like structure with PUA aggregates coated with and wrapped in PVdF-HFP rich surface films. However, PUA-FS has a higher PVdF-HFP content and less PUA content than PUA-EC, since the free-standing membrane requires sufficient mechanical strength. Hence, PUA-FS is less conductive than PUA-EC; 4.9104 S cm1 in contrast to 5.7104 S cm1 at 30 C.
The solid-state battery is assembled with lithium iron phosphate (LFP) as the cathode, lithium metal foil as the anode, and PUA-FS or PUA-EC as electrolyte. Galvanostatic charge/discharge cycles are performed at room temperature between 2.0 - 4.0 V, with charging current 0.1 C, 0.2C, 0.3C, and 0.5 C at 100% depth of discharge. The PUA-FS battery is evidently superior to the PUA-EC battery in cycle stability and rate capacity. For the PUA-FS battery, the maximum capacity at 0.1C is 169.7 mAh g-1, the capacity loss is 0.036% per cycle, and the current cycle number exceeds 250. The maximum capacity at 0.3C is 147.0 mAh g1, the capacity loss is 0.069% per cycle, and the current cycle number exceeds 600.

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