全固態鋰金屬電池 (All-solid-state lithium metal battery, ASSLB) 具備高安全性和高能量密度的優勢，被視為下個世代最具發展潛力的儲能裝置。尤其軟包電池可以透過正極 | 隔離膜 | 負極重複堆疊進而達到提升能量密度的能力，儼然在現今成為商業及學界中的主流發展。然而，ASSLB面臨了許多挑戰，包括固態電解質 (Solid electrolyte, SE) 的不穩定、固體介面間的高阻抗以及受限於製膜工藝而影響到電池規模…等，從內部反應到外部組裝都仍然有待解決。
本研究首先針對軟包電池膜的製備及組裝製程的部分進行探討。跟隨實驗室內製膜工藝的發展，使用可脫式片狀膜的技術，利用具可分離特性之高分子的基材，將塗佈好的SE (隔離膜) 獨立分離使用，從而單獨控制隔離膜的面積大小，加以利用對於各材料面積的控制，完整使用正極內的活物。再來為軟包電池組裝完成後堆疊壓力 (Stack pressure) 及加壓材料的選用，以一連串實驗確立使用40 MPa的堆疊壓力以及使用訂製鋼板作為加壓材料，最後添加以冷均壓 (Cold isostatic press, CIP) 施加製程壓力 (Fabrication pressure) 的步驟，將軟包電池的組裝標準化，供往後實驗室研究人員為用。
研究第二個主軸是對ASSLB的一些參數進行測試，探討這些參數對於電池表現的影響。首先壓力的影響，發現製程壓力的增加對於電性的提升呈現正向關係，但堆疊壓力卻必須加壓到某種程度，才會在電性表現上有展現。此外，溫度對於消弭電池阻抗也有很顯著的影響，但阻抗卻會在降溫後再度上升，本實驗在55˚C的升溫環境下的軟包電池，展現出172.9 mAh/g的充電電容量，高於升溫前的電容量將近兩倍。鹵化物/硫化物雙夾層的應用，成功阻隔彼此對於正負兩極的介面反應，以雙夾層系統所組裝的軟包電池在55 ˚C的升溫環境下能夠擁有185 mAh/g的可逆電容量及82.65% 的首圈庫倫效率。由不同比例導電碳的實驗也證明得知，增加導電碳比例可以有效提升正極內導電度，減緩整體電池的極化現象，並獲得更高的正極使用率。最後為無溶劑式複合正極的應用，正極內均勻的導電碳分佈讓活物的利用率提升，並且展現出206.3 mAh/g的首圈充電電容量及79.34% 首圈庫倫效率。
結合以上製程及介面間的測試，對於提升ASSLB的能量密度的目的又更進一步，即使對於使用高容量複合正極的電池仍有待探討，但卻為此領域的研究建立起一個具參考價值的平台。

As one of the next generation’s most promising and crucial energy storage devices, all-solid-state lithium-ion batteries (ASSLBs) are renowned for their safety and high energy density. In addition, pouch cell has become mainstream due to its capability of stacking electrodes. However, the solutions to challenges that ASSLBs have faced, including instability of the solid electrolyte (SE), high interfacial impedance resulting from solid contacts, and limited scalability concerning film fabrication, are still not being widely addressed.
This work first focuses on the fabrication of films and the assembly process of pouch cells. As the fabrication technique progressed in the lab, a freestanding film was demonstrated by using a polymer substrate with the property of getting separated to control the size of the SE (separator) independently. It’s allowed for precise control over the area of the separator and achievement for full utilization of the active materials in the cathode. Furthermore, stack pressure and compression materials are selected by going through a series of experiments, finally, with a stack pressure of 40 MPa and customized steel plates as the compression material. Lastly, an instrument, a cold isostatic press (CIP), is introduced to apply fabrication pressure, establishing the standard process for assembling pouch cells for future research in the lab.
The second part of the study is to test various parameters of ASSLBs and investigate their impact on battery performance. The influence of pressure shows a positive correlation between fabrication pressure and electrochemical performance. However, stack pressure somehow shows a threshold effect, requiring a certain pressurization level to impact the cell further. In addition, temperature also has a significant effect on reducing battery interfacial impedance, which tends to increase again after cooling down. The pouch cell cycling under a heated environment at 55˚C has a charging capacity of 172.9 mAh/g, nearly double the capacity before heating. The configuration of a halide/sulfide bilayer has successfully prevented interfacial side reactions with the negative and positive electrodes, respectively, allowing the bilayer system to achieve a reversible capacity of 185 mAh/g and 82.65% for the first coulombic efficiency under a heated environment at 55˚C. Furthermore, increasing the proportion of conductive carbon in the composite electrode to improve the electronic conductivity successfully mitigated the overall polarization of the battery. Lastly, solvent-free composite cathodes with uniform distribution of conductive carbon led to better active material utilization, showing the first charging capacity of 206.3 mAh/g and the first coulombic efficiency of 79.34%.
With the improvement of the assembly process and interfacial analysis mentioned above, the goal of increasing the energy density of ASSLBs is getting closer. Although further exploration is required for batteries with high-loading composite cathodes, this study has established a valid platform for ASSLBs.

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