本論文提供一快速、低成本、高離子含量、具自修復效果、高 電導率，以常見有機溶劑即可溶解之鋰電池固態電解質之新型合成 策略。本篇使用 2-丙烯醯胺基-2-甲基丙磺酸 (2-acrylamido-2- methylpropane sulfonic acid, AMPS) 作為陽離子單體，行諾里什Ⅰ型光 化 學 反 應 (Norrish type I reaction) 合成兩種系列共聚物 (PAMPLEO1AA、PAMPLEO3AA)。藉由調控陽離子單體 AMPS 及單體共聚物莫耳比，可開發出高分子 PAMPLEO3AA (目前 PAMPLEO3AA 已開發出 AMPS 莫耳百分比為 50%、離子含量 74% 之比例)，後續添加重量百分比 55 wt% 之聚偏二氟乙烯 ( polyvinylidene difluoride, PVDF )，及 18 wt% 之鋰鹽 LiTFSI 製備 固態電解質 AMPBL632，應用於 NCM811 電池進行各項參數研究。 此外物性測試部分 PAMPLEO1 以 80 °C 加熱後於 6 小時顯現出自修復效果。並且由量測結果後得知 PAMPLEO3AA 帶有一定防火性， 且具十足之熱穩定性。藉由量測後得知 AMPBL632 其鋰離子遷移數 tLi+ 量測可達 0.42，並且於 25 mA/g 電流密度下進行循環充放電測試 展現出 35.45% 之庫倫效率。其電化學窗口可達 4.99V vs Li/Li+，且 其電導率可達驚人的 5.18 × 10−4 Scm-1 高數值，其有望應用於高壓鋰 ii 電池並具優異之效能。後續機械應力及 SEM 皆驗證對於固態電解質 而言，PAMPLEO3AA 的加入可有效提升其機械應力及產生鈍化層 的作用，應可有效保護電極不受氧化還原影響導致崩解。部分結果 已可說明 PAMPLEO3AA 之材料具備非常優越之性能，且對應用於 鋰電池之聚合物單離子固態電解質提供一種新思路，乃非常具有未 來展望性之新型電解質。;This study provides a new strategy for the cost-effective synthesis of PAMPL based polymers which show highly ionic, self-healing, and high electrical conductivity properties. Gratifyingly, the synthesized polymers are well soluble in common organic solvents. The synthesis of PAMPL polymers (PAMPLEO1AA and PAMPLEO3AA) were achieved by the Norrish type I reaction of anionic monomer viz 2-acrylamido-2- methylpropane sulfonic acid (AMPS) and copolymonomer. Physical property test for self-healing of PAMPLEO1 revealed that PAMPLEO1 confirm self-healing at 80oC in 6h. In addition, the PAMPLEO3AA was also confirm fire-resistence property and thermal stability. Moreover, the synthesis of the solid polymer electrolyte AMPBL632 was achieved by the addition of 55 wt% of polyvinylidene (PVDF) and 18 wt% LiTFSI to PAMLEO3AA (50% AMPS, 74% ionic monomer) polymers. AMPBL632 produced the highest lithium transference number (tLi+) up to 0.42. Further, the AMPBL632 achieved 35.45% coulombic efficiency after 5 cycles at 25mA/g current density. Delightfully, the high electrochemical window up to 4.99V of AMPBL632 could be the potential for high voltage lithium battery. In addition, the ion conductivity test of AMPBL632 generated the conductivity up to 5.18 × 10−4 Scm-1. The mechanical stress and scanning electron microscope proved the addition of PAMPLEO3AA the electrolyte to PVDF would promote the higher mechanical stress, and it also produced passive layer which was efficiently protecting the electrode during the redox reaction. The above-mentioned properties confirmed that PAMPLEO3AA would be a superior performance in Li-batteries over AMP electrolyte Li-batteries. Thus, PAMPLEO3AA will be absolutely a future prospect single-ion solid polymer electrolyte.
