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研究生： 王鴻銘
Hong-Ming Wang
論文名稱： 新型態鋰離子電池添加劑(硫脲嘧啶/雙馬來醯亞胺)之研究探討
The investigation of new type of additive(2-thiouracil and N,N’-bismaleimide-4,4’-diphenylmethane) in lithium-ion battery
指導教授： 陳崇賢
Chorng-Shyan Chern
口試委員: 許榮木
JUNG-MU HSU
范國泰
Quoc-Thai Pham
學位類別： 碩士
Master
系所名稱： 工程學院 - 化學工程系
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： 113
中文關鍵詞： 鋰離子電池 、添加劑 、硫脲嘧啶 、雙馬來醯亞胺
外文關鍵詞： lithium-ion battery, additive, 2-thiouracil, N,N’-bismaleimide-4,4’-diphenylmethane
相關次數： 點閱：492  下載：0 
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    • 本研究的第一部分探討不同莫耳比之硫脲嘧啶/雙馬來醯亞胺(TUR/BMI)添加劑的反應機制類型，添加HQ抑制劑後得知TUR/BMI = 1/2的自由基加成聚合反應比例高於TUR/BMI = 1/1，接著利用差示掃描量熱法(DSC)分析聚合反應程序所需的反應溫度以及反應熱，同時以自由模型法計算活化能，再藉由熱重分析(TGA)測量所製備之添加劑的熱穩定性，得知添加劑內的BMI含量越高可提升材料的耐熱性質。
    第二部分則將不同莫耳比之硫脲嘧啶/雙馬來醯亞胺(TUR/BMI)添加劑應用於鋰離子電池，同時為了解硫 脲嘧啶與脲嘧啶(UR)在電性表現上的差異，本研究以循環伏安法(CV)、充放電測試以及交流阻抗圖譜(EIS)等測試方法來探討所製備之添加劑對於正極材料LiNi0.5Co0.2Mn0.3O2 (NCM523)的影響。在實驗結果的部分，得知TUR/BMI = 1/1_0.5 %可有效改善常溫下充放電的電性表現，而在高溫(55 ℃)條件下的充放電測試中TUR/BMI = 1/2_0.5 %有較佳的電性表現，顯示過量的雙馬來醯亞胺(BMI)可有效改善正極半電池對高溫的耐受性，至於在不同充放電速率的測試結果，得知TUR/BMI在不同添加量的電性表現皆是優於UR/BMI。

    The first part of this study investigates the reaction mechanisms of 2-thiouracil/N,N’-bismaleimide-4,4’-diphenylmethane (TUR/BMI) additives with different molar ratios. After adding HQ (inhibitor), TUR/BMI = 1/2 shows the higher degree of free radical reaction than TUR/BMI = 1/1. Then, differential scanning calorimetry (DSC) is used to analyze the reaction temperature and reaction heat for the process of polymerization. Furthermore, the model free method is used to determine the activation energy for the polymerization of BMI with TUR. With thermogravimetric analysis (TGA), the thermal stability of additives can be enhanced by increasing the content of BMI.
    In the second part, TUR/BMI as the additives with different molar ratios are applied to lithium-ion battery. Also, this study will compare the difference between TUR and uracil (UR). Cyclic voltammetry (CV), charge and discharge tests and electrochemical impedance spectroscopy (EIS) are used to analyze the effect of the additives on the cathode material LiNi0.5Co0.2Mn0.3O2. The experimental result shows that TUR/BMI = 1/1_0.5 % can effectively improve the cycle stability at room temperature. In addition, it can be clearly seen that TUR/BMI = 1/2_0.5 % has better electrochemical performance than other additives at high temperature. This result indicates that excessive BMI can enhance the high temperature resistance. As for the C-rate test, different amounts of TUR/BMI additives exhibit better rate capability than UR/BMI.

    摘要 I Abstract II 目錄 III 圖目錄 VI 表目錄 XI 第一章 緒論 1 1.1 前言 1 1.2 研究背景 2 1.2.1 鋰離子電池工作原理 2 1.2.2 正極材料 2 1.2.3 隔離膜 4 1.2.4 電解液 5 1.2.5 負極材料 5 1.3 鋰離子電池之熱失控 6 第二章 文獻回顧 8 2.1 改善鋰離子電池安全性之方法 9 2.1.1 隔離膜改質 9 2.1.2 電解液改質 15 2.1.3 正極材料之塗層技術 19 2.1.4 正極材料摻雜其他金屬元素 23 2.1.5 正極材料添加劑 27 2.2 寡聚物添加劑之聚合加成反應類型 33 2.1.1 Free radical polymerization 34 2.1.2 Aza-Michael addition reaction 36 2.3 研究動機與目的 37 第三章 實驗藥品、儀器與方法 38 3.1 實驗藥品 38 3.2 實驗儀器 39 3.3 實驗方法 40 第四章 結果與討論 46 4.1 LIVING@添加劑DSC分析 46 4.1.1 TUR/BMI = 1/1 46 4.1.2 TUR/BMI = 1/2 47 4.2 LIVING@添加劑反應機制探討 49 4.3 LIVING@添加劑動力學分析 51 4.3.1 TUR/BMI = 1/1 52 4.3.2 TUR/BMI = 1/2 53 4.4 LIVING@添加劑之NMR結構分析 55 4.4.1 TUR/BMI = 1/1 55 4.4.2 TUR/BMI = 1/2 57 4.5 LIVING@添加劑DLS粒徑分析 59 4.6 LIVING@添加劑TGA分析 60 4.7 電化學性能分析 62 4.7.1 循環伏安(CV)分析 62 4.7.2 第一圈充放電曲線分析 68 4.7.3 常溫充放電循環測試 69 4.7.4 常溫LIVING@添加劑之充放電曲線 71 4.7.5 常溫LIVING@添加劑之交流阻抗圖譜分析 73 4.7.6 高溫(55 ℃)充放電循環測試 76 4.7.7 高溫(55 ℃)LIVING@添加劑之充放電曲線分析 78 4.7.8 高溫(55 ℃)LIVING@添加劑之交流阻抗圖譜分析 80 4.7.9 不同充放電速率之電性表現 82 4.8 電極極片SEM分析 85 第五章 結論 88 第六章 參考文獻 89 附錄 98

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