臺灣博碩士論文加值系統

本研究以現有鋰電池產線為基礎，不須更改設備和製程，透過注液方式將開發之膠態電解質注入鋰電池中，能得到具高安全性之鋰電池。此膠態高分子電解質以聚丙烯腈(Poly(acrylonitrile-co-methyl acrylate)，PAN-MA)高分子為主架構，混摻聚乙二醇(Poly(ethylene glycol)，PEG)高分子，加入商用液態有機電解液(LE; 1M LiPF6 in EC/DMC=1/1 v/v)中，加熱攪拌至高分子完全溶解呈均勻相，靜置一段時間後會自凝成膠轉變為果凍狀之膠態高分子電解質(GPE)，具現址成膠能力。
藉由Raman分析、導離子度量測、黏度測試、介電譜分析、鋰離子遷移常數(0.62)分析與電化學穩定電位窗(~5.3 V)測量，得知GPE因加入高分子，存在鋰鹽-高分子作用力，能促進鋰鹽完全解離，雖然黏度比LE稍高，但仍不影響鋰電池電解質注液過程，且高分子能與溶劑化鋰離子產生作用力，藉由自身的鏈段運動傳遞鋰離子，並同時吸引PF6-減少離子基團團聚，相對LE而言，上述性質有助於提升系統的導離子度和鋰離子遷移數，還能避免鋰鹽電化學分解反應的進行，進而提升膠態高分子電解質的電化學穩定電位窗。
而在電池性能表現方面，使用磷酸鋰鐵正極搭配鋰金屬負極，並選擇用於超級電容器中的cellulose作為隔離膜，以LE與GPE組裝成2032鈕扣型電池進行測試及比較差異。在室溫25 ℃及0.1 C-rate的放電速率下，GPE電池擁有164 mAh/g之高電容量，在15 C-rate的放電速率下仍擁有22 mAh/g之電容量，遠遠優於LE電池(0.1 C-rate具有158mAh/g之電容量；13 C-rate具有9 mAh/g之電容量)。將電池進行長效充放電測試，以1 C-rate充電、5 C-rate放電，循環充放電300圈後，GPE鋰電池電容維持率仍有83 %。最後進一步組成軟包電池做可行性和安全性測試，發現不論是彎折、剪斷都未影響電池放電能力，且未發現有任何電解質滲漏的情況發生，故我們可以利用此系統自凝成膠之特性，應用在現有鋰電池生產線中，不需投入資金更改設備和製程，即可生產不會發生漏液且具高效能、高安全性之膠態鋰電池。

關鍵字：鋰電池、膠態高分子電解質、聚丙烯腈、自凝成膠

This study incorporates polymer into commercial liquid electrolyte (LE) to form gel polymer electrolyte (GPE) which exhibits auto-gelation after standing for a while. The GPE comprises polyacrylonitrile-co-methyl acrylate (PAN-MA) blending polyethylene glycol (PEG) as a host dissolved by a LE of 1 M LiPF6 in a carbonate solvent. The battery which used GPE exhibits high safety and excellent performance because its polymer chain would interact with Li-EC complexes and facilitate Li-ion migrate. Also, it has interaction with PF6− anions to effectively disperse the cluster ions and decreased the solvation degree of Li+ that accelerate the transport of Li+ ion. As a result, GPE exhibits high ionic conductivity (1.72×10-3 S/cm at room temperature) , a wide electrochemical window of 5.3 V (vs. Li/Li+) and high lithium ion transfer number (0.62). The battery assembled using GPE, i.e., Li/GPE/LiFePO4, delivering a capacity of 164 mAh·g-1 at 0.1 C-rate and 22 mAh·g-1 at 15 C-rate. The most important is GPE in this study can be applied in battery industrial process without any equipment change, and the flexibility is helpful for application in various sizes of electronic devices. That mean, we can manufacture high safety lithium batteries which could fully avoid electrolyte leakage by existing battery factories.

Keywords：Lithium battery, Gel polymer electrolyte, Poly(acrylonitrile), Auto-gelation

中文摘要 I
英文摘要 III
誌謝 X
本文目錄 XII
表目錄 XV
圖目錄XVI
第一章 緒論 1
1-1前言-電池發展與介紹 1
1-2 鋰電池與鋰離子電池 3
1-2-1裝置構造 4
1-2-2工作原理 4
1-3電極材料 6
1-3-1正極材料 6
1-3-2負極材料 10
1-4電解質 12
1-4-1液態有機電解質 13
1-4-2膠態高分子電解質 15
1-4-3固態高分子電解質 16
1-4-4無機固態電解質 19
1-5常見鋰離子電池專有名詞與計算 21
1-5-1理論電容量計算 21
1-5-2專有名詞介紹 22
1-5-3電池組串並聯計算 23
1-6全球鋰電池商業概況 25
1-7研究動機與目的 29
第二章 理論說明與文獻回顧 31
2-1 聚丙烯腈性質與回顧 31
2-2 導離子度 33
2-3 正離子遷移常數 35
第三章 實驗方法與儀器原理介紹 38
3-1 實驗藥品 38
3-2 實驗儀器設備 39
3-3 磷酸鋰鐵(LiFePO4)正極之極片製作 41
3-4 石墨(graphite)負極之極片製作 41
3-5 膠態高分子電解質製備 42
3-6鈕扣型電池(coin-cell)組裝 43
3-7軟包鋰電池製作 44
3-8實驗分析儀器與裝置分析儀器原理簡介 45
3-9電化學測試 50
3-10電池性能測試 52
3-11實驗流程 53
第四章 結果與討論 54
4-1 膠態高分子電解質物理化學分析 56
4-1-1隔離膜與膠態高分子電解質形貌 56
4-1-2 SEM分析 57
4-1-3熱穩定性分析 58
4-1-4 Raman分析 59
4-2 膠態高分子電解質電化學分析 62
4-2-1離子傳導度(Ionic conductivity, σ) 62
4-2-2鋰離子遷移數(Lithium transference number, tLi+) 66
4-2-3電化學穩定度量測 69
4-3 電池性能測試 71
4-3-1 LiFePO4電池充放電測試 71
4-3-2電池短路性能測試 75
4-4 軟包裝鋰電池安全性測試 76
4-5 介電常數測試 77
4-6 文獻比較 80
第五章 結論與建議 81
參考文獻 82

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