本研究利用自由基聚合法製備交聯結構之聚醚高分子，以直接塗佈於磷酸鋰鐵電極表面的方式進行聚合反應，製備擬固態高分子電解質應用於鋰金屬電池中。在TGA與DSC分析中發現，交聯高分子主體具有良好的熱穩定性，藉由改變主結構的高分子混合比例，能夠降低系統的結晶性，有助於鋰離子的傳遞；其離子傳導度在60℃可達1.31×10-3 S cm-1、電化學穩定視窗可達5.2 V且具有良好的電化學可逆性，而鋰離子遷移率更高達約0.6。於鋰金屬電池充放電效能測試中亦有優良的表現，在3C放電速率下可保有91.3 %的電容維持率(相對於0.1C )，在長效循環充放電120圈後仍有91.9%的電容維持率，庫倫效率維持於98% 以上，但由於塑化劑與鋰金屬所具有的反應性，使得電池於循環充放電200圈後電容維持率降至76.1%。後續進一步導入無機材料製備複合性高分子電解質，於離子傳導度測試中發現混摻無機材料後傳導度值確有增加，但混摻比例不宜過高，會造成界面阻抗增加與極化現象的加劇。導入SiO2材料後雖然造成快速充放電效能有所下降，但能夠提高電解質系統的穩定性，將長效循環充放電200圈的電容維持率提升至85.8%。經由SEM影像觀察充放電後鋰金屬表面與截面，相較於一般液態電解質生成明顯鋰支晶層，使用本研究之固態高分子電解質則無明顯鋰支晶生成，於鋰金屬表面產生平整之SEI層。由以上所述可歸納本研究所製備固態高分子電解質具備優異的電化學特性，亦能夠抑制鋰支晶的生成，可應用於鋰金屬電池系統。

We synthesized the cross-linked network polyether-based polymer electrolytes through the free-radical polymerization. By direct coating the polymer electrolytes on the cathode surface, we obtain quasi-solid-state polymer electrolytes for lithium metal batteries. The TGA and DSC analysis show that the cross-linked polymer backbone have good thermal stability. We can decrease the crystallinity by changing the ratio of the cross-linker and mono-functional polyether, which can enhance the mobility of lithium ions. The polymer electrolytes exhibit high ion conductivity (1.31×10-3 S cm-1, at 60oC), good electrochemical stability (onset potential ~ 5.2V ) and the highest lithium transference number can reach about 0.6 . Of particular important is that the excellent capacity retention at the high discharge current (3C) can achieved 91.3% ( compare to 0.1C ). It also can endure long charge/discharge cycling. After 120 cycling, the capacity retention is 90.9% compare the initial one and keep the coulombic efficiency above 98%. Unfortunately, the capacity retention decay to 76.1% after 200 cycling because the poor compatibility of plasticizer and lithium metal.
In order to improve the cyclic performance, we introduced the non-organic fillers to obtain the composite polymer electrolytes. The ionic conductivity enhances by adding small amount of fillers. However, the polymer electrolytes would increase the interfacial resistance and the polarization when the dosage of fillers is more than 1%. The most significant improvement is that the retention can keep 85.8% after 200 cycling by adding SiO2 nanofillers. In addition, compared to the commercial liquid electrolytes, lithium dendrites formed ununiformed and roughness on the lithium metal surface after charge/discharge. The cross-linked polymer electrolytes show good ability to suppress the growth of lithium dendrites and stabilize the passivation layer. All the above-mentioned properties indicate that the cross-linked polymer electrolytes can be a good candidate of lithium metal batteries.

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