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研究生： 林宇杏
Lin, Yu-Hsing
論文名稱： 雙鹽雙高分子設計之膠態電解質應用於鋰電池
Gel Electrolyte with Dual-salt and Dual Polymer Design for Lithium Batteries
指導教授： 鄧熙聖
Teng, Hsisheng
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年： 2020
畢業學年度： 108
語文別： 中文
論文頁數： 101
中文關鍵詞： 鋰電池 、膠態高分子電解質 、聚偏二氟乙烯 、雙鋰鹽
外文關鍵詞： Lithium battery, Gel polymer electrolyte, PVDF-co-HFP, Dual salt
相關次數： 點閱：77  下載：0 
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    • 鋰金屬電池擁有高能量密度，在儲能系統上有相當大的潛力，然而使用傳統的液體電解質難以建立穩定的固體電解質介面層（SEI layer）和抑制鋰枝晶生長。本研究以聚偏二氟乙烯(Polyvinylidene fluoride，PVDF)高分子為主架構，混雜聚甲基丙烯酸羥乙酯(Polyhydroxyethylmethacrylate，PHEMA)高分子，溶於商用液態電解液中，並同時引入雙鋰鹽(LiTFSI-LiPF6)系統，旨在解決介面層與鋰枝晶的問題，加熱攪拌至均勻相，並注入Celgard商用隔離膜，靜置一段時間後會轉變為果凍狀之膠態電解質。
    此膠態電解質於室溫下具有高導離子度(1.1×10-3 S cm-1)、寬廣的電位窗(5.0 V)，通過量測膠態與液態電解質阻抗隨時間的變化，及SEM、XPS量測鋰金屬表面，去證明此膠態電解質可以形成穩定的SEI層及抑制鋰枝晶。電池性能表現方面，使用磷酸鋰鐵正極搭配鋰金屬負極，組裝成2032鈕扣型電池，於室溫(25℃)下，以0.1 C-rate的放電速率，膠態電解質擁有165 mAh g-1的電容量，以17 C-rate的高速放電速率下仍保有64 mAh g-1的電容量，遠優於液態電解質(0.1 C-rate具有160 mAh g-1的電容量，17 C-rate具有7 mAh g-1的電容量)。長效循環充放電測試下，以1C-rate進行循環充放電500圈後，電容維持率仍大於90%。電池安全性測試的部分，以0.5 mA cm-2 電流下進行500小時的短路測試，都仍未有短路的現象發生，另外，將膠態電解質製作成軟包電池，經剪斷、彎折都未發現有電解質漏液的現象發生，可見其具有一定的安全性。此自凝成膠膠態電解質具有抑制鋰枝晶及優異的充放電性能，可應用在現今的鋰電池產線。

    Lithium metal batteries (LMBs) which have high energy density are promising candidate for next-generation batteries. However, it is difficult to build a stable solid electrolyte interface layer (SEI layer) and inhibit the growth of lithium dendrites using traditional liquid electrolytes. Herein, a gel electrolyte with dual-salt (LiTFSI-LiPF6) and dual polymer (PVDFcoHFP-PHEMA) design is developed for stabilize the interfacial contact between electrode and electrolyte. The gel electrolyte matrix with a physical network can regulate the anions to promote lithium ion transportation. The resulting gel polymer electrolyte presents an extremely high lithium‐ion transference number of 0.6 and ionic conductivity (1.1×10-3 S cm-1). More significantly, the synergistic effect from the dual polymer and dual salt enabling stable ion deposition effectively suppresses the growth of lithium dendrites. Armed with the GPE, stable symmetric Li/Li cells demonstrate a long cycle life of 500 h at a high current density of 1 mA cm−2 and no sign of lithium dendrite. In terms of the charge and discharge performance of battery, GPE which is assembled into Li||LiFePO4 batteries, exhibited superior capacity, high rate retention, and cycling stability. This gel electrolyte not only can basically solve the problem of LMBs but also directly apply on the current battery assembly line.

    總目錄 中文摘要 I 英文摘要 II 誌 謝 XIII 總目錄 XV 表目錄 XIX 圖目錄 XX 第一章 緒論 1 1-1 電池的發展與介紹 1 1-2 鋰離子電池 3 1-2-1 裝置構造 4 1-2-2 工作原理 5 1-3 電極材料 6 1-3-1 正極材料 6 1-3-1-1 磷酸鋰鐵LiFePO4 (LFP) 6 1-3-1-2 三元正極材料 (NMC、NCA) 7 1-3-1-3 鋰鈷氧化物 (LCO) 9 1-3-2 負極材料 10 1-3-2-1 碳材負極 11 1-3-2-2 過渡金屬氧化物負極(鈦酸鋰Li4Ti5O12) 12 1-3-2-3 合金負極材料 13 1-4 電解質 15 1-4-1 液態電解質 15 1-4-2 膠態高分子電解質 18 1-4-3 固態電解質 21 1-5 常見鋰離子電池專有名詞 27 1-5-1 理論電容量計算 27 1-5-2 專有名詞介紹 28 1-6 全球鋰電池商業概況 29 1-7 研究動機與目的 31 第二章 理論說明與文獻回顧 32 2-1 聚(偏二氟乙烯-co-六氟丙烯)，PVDF-HFP 32 2-2 聚甲基丙烯酸羥乙酯，PHEMA 34 2-3 雙鋰鹽系統電解質 35 2-4 導離子度 36 2-5 鋰離子遷移常數 38 第三章 實驗方法與儀器原理介紹 41 3-1 實驗藥品與用品 41 3-2 實驗儀器設備 42 3-3 磷酸鋰鐵(LiFePO4)正極之極片製作 43 3-4 石墨(Graphite)負極之極片製作 43 3-5 雙鋰鹽雙高分子膠態電解質製備 44 3-6鈕扣型電池(coin-cell)組裝 45 3-7 實驗分析儀器與裝置分析儀器原理介紹 46 3-7-1 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 46 3-7-2 X射線光電子能譜 (X-ray Photoelectron Spectroscopy, XPS) 48 3-7-3 拉曼光譜分析(Raman Spectrum) 49 3-8 電化學測試 51 3-8-1 導離子度 (Ionic conductivity, σ) 51 3-8-2 線性掃描伏安法(Linear sweep voltammogram, LSV) 52 3-8-3 鋰離子遷移常數 (Lithium transference number, tLi+) 52 3-9電池性能測試 52 第四章 結果與討論 53 4-1 雙鹽雙高分子膠態電解質物性化性分析 54 4-1-1 Celgard隔離膜與雙鹽雙高分子膠態電解質的結合 54 4-1-2 膠態高分子電解質的SEM分析 56 4-1-3 Raman 分析 57 4-2 雙鹽雙高分子之膠態電解質電化學分析 60 4-2-1 導離子度（Ionic conductivity, σ） 60 4-2-2 鋰離子遷移數（Lithium transference number, t_(〖Li〗^+ )） 64 4-2-3 電化學穩定度量測 66 4-3 電池性能量測 69 4-3-1 電池充放電測試 69 4-3-2 電池長效循環充放電測試 74 4-3-3 電池短路性能測試 76 4-4 儀器分析(鋰金屬測試) 77 4-4-1 X射線光電子能譜測試 77 4-4-2 掃描式電子顯微鏡測試 80 4-4-3 EIS測試 82 4-5 軟包電池性能測試 83 4-5-1 軟包電池安全性測試 83 4-5-2 軟包電池充放電測試 83 4-6文獻比較87 第五章 結論 88 參考文獻 89

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