固態鋰電池（SSLB）可作為克服傳統液態電解質型鋰離子電池局限性的解決方案，例如增強安全性、提高能量密度和更廣泛應用可能性的優勢。然而，廣泛採用SSLB面臨須開發具有卓越離子導電性和鋰離子傳輸數的固態聚合物電解質（SPE）相關的重大挑戰。本論文匯總兩個部分的研究結果，對高性能SSLB的關鍵挑戰提供了創新策略。 第一部分研究藉由引入β-氰基醚基和丙烷磺酸醚基改質聚乙烯醇（PVA），提高SPE的離子導電性並實現固態鋰電池優良的充放電循環性能。當這種新型接枝聚合物與50 wt%的三氟甲磺醯亞胺鋰（LiTFSI）相結合時，離子導電率為5.4×10-4 S cm-1和31.6 kJ mol-1的低活化能。值得注意的是，電化學穩定視窗達到5.3 V（相對於Li/Li+），在室溫（約25 °C）下鋰離子遷移常數為0.48。Li|SPE|Li電池在500次循環中沒有短路，並且固態Li|SPE|LiFePO4電池表現出卓越的循環穩定性，在0.5 C速率下576個循環後克電容量138 mAh g−1，電容量維持率為70%。
至於第二部分則著重於合成聚（乙二醇）甲醚丙烯酸酯（PEGMEA）功能化的磺基甲基丙烯酸酯（SBMA）藉以改善其電化學和機械性能。PEGMEA單元作為降低玻璃化轉變溫度的軟鏈段，而SBMA單元則作為增加Li+遷移性的單元。藉由將共聚物與50 wt%的LiTFSI混合製備SPE，表現出最大離子導電率為19.3×10–5 S cm–1，鋰離子遷移常數為0.31，並在室溫下具有5.23 V的氧化電位穩定性。選定的SPE被引入到SSLB中，在0.1 C速率下的比電容量為169 mAh g–1和在0.5 C速率下的比電容量為146 mAh g–1，經過450個循環後仍然能獲得電容量維持率在70%。值得注意的是，共聚物的SPE更優於採用單一聚合的SPE的電池表現，此結果顯示藉由這種創新共聚物設計實現的卓越電化學性能。
這篇論文全面概述了固態鋰離子電池的最新進展。探討了新型SPE材料的合成、物理化學性質和電化學性能，為它們在未來可持續鋰離子電池和綠能能源技術中的潛力提供了光明的前景。本論文不僅有助於對這些先進材料的理解，還強調了它們在SSLB的持續演進中的關鍵作用，為更安全、更高效和環保的能源儲存解決方案提供了一個方向。

Solid-state lithium batteries (SSLBs) have emerged as a promising solution to overcome the limitations of conventional liquid electrolyte-based lithium-ion batteries, providing enhanced safety, increased energy density, and broader application possibilities. However, the widespread adoption of SSLBs faces significant challenges related to the development of solid polymer electrolytes (SPEs) with superior ionic conductivities and lithium transference numbers. This thesis consolidates the findings of the pursuit of high-performance SSLBs. The first part investigates the modification of polyvinyl alcohol (PVA) through the incorporation of β-cyanoethyl ether and propanesulfonate ether groups, in a concerted effort to enhance the ionic conductivity of SPEs and achieve satisfactory cycling performance for solid-state lithium batteries. When this novel graft-polymer was combined with 50 wt% of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), it was demonstrated a remarkable ionic conductivity of 5.4×10-4 S cm-1, accompanied by a low activation energy of 31.6 kJ mol-1. Notably, the electrochemical stability window reaches 5.3 V (vs. Li/Li+), and the lithium transference number of 0.48 at room temperature (approximately 25 °C). The Li|SPE|Li cell undergoes 500 cycles without short-circuiting, and a solid-state Li|SPE|LiFePO4 battery demonstrates exceptional cycling stability, achieving a discharge capacity of 138 mA h g−1 at 0.5 C-rate and capacity retention of 70% after 576 cycles.
The second part focuses on the synthesis of poly(ethylene glycol) methyl ether acrylate (PEGMEA) functionalized with sulfobetaine methacrylate (SBMA) pendants to enhance electrochemical and mechanical properties. The PEGMEA unit, serving as a soft segment to decreasing the glass transition temperature, while the SBMA unit functions as a zwitterionic unit to increasing Li+ mobility. SPEs were prepared by mixing copolymers with 50 wt% of LiTFSI and it exhibits a maximum ionic conductivity of 19.3×10–5 S cm–1, a lithium transference number of 0.31, and an oxidation stability of 5.23 V at ambient temperature. The selected SPE is incorporated into a SSLB, yielding a discharge capacity of 169 mA h g–1 at 0.1 C-rate and 146 mA h g–1 at 0.5 C-rate, maintaining a capacity retention of 70% after 450 cycles. Notably, the copolymer-based SPEs outperform a reference battery with a homopolymer-based SPE, emphasizing the superior electrochemical properties achieved through this innovative copolymer design.
This thesis provides a comprehensive overview of recent advancements in solid-state polymer electrolytes for SSLBs. It explores the synthesis, characterization, and electrochemical performance of these novel SPE materials, shedding light on their potential for revolutionizing the future of sustainable lithium batteries and clean energy technologies. The thesis not only contributes to the understanding of these advanced materials but also underscores their critical role in the continued evolution of SSLBs, offering a path towards safer, more efficient, and environmentally friendly energy storage solutions.

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