岐狀結構材料在鋰電池的應用

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姓名

李昱翰(Yu-han Li) 查詢紙本館藏

畢業系所

化學學系

論文名稱

岐狀結構材料在鋰電池的應用
(The applications of hyperbranched on Li ion batteries)

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摘要(中)

我們以雙酮衍生物為起始劑來製備雙馬來亞醯胺高分歧狀寡聚物。並探討其成長機制以及起使劑衍生物、反應時間等對離子動力學的影響。以雙酮衍生物為起始劑能夠有效的增加反應的轉化率而且能夠使其在較低的溫度下進行反應，增進了高分歧狀寡聚物的應用性。
再者，我們設計了具有高度運動性之高分歧狀寡聚物應用於電池添加劑。由研究發現帶來電池循環穩定性以及安全性上升，特別是在55℃的高溫循環壽命，另外，也降低了電池的放熱量以及溫度，使電池內短路測試之溫度由700℃之高溫下降至85℃，大幅度提升了電池的安全性。此高分歧狀寡聚物確實可用來作為安全性添加劑，並且滿足了高性能高安全性鋰電池的應用。

摘要(英)

In this research, we use Diketone derivatives as initiator to prepare Bismaleimide-based Hybranched oligomer and also investigate the propagation mechanism、dynamic characters of Bismaleimide-based Hybranched oligomer affect by the ratio of initiators and the reaction time. The Diketone derivative as initiator can promote the conversion rate. It provides a better ways to promote the conversion rate of Bismaleimide at low temperature (130℃). These findings should be useful for practical application .
Furthermore, we used the Hyperbranched oligomer as additive in the electrolyte to improve the safety features in lithium battery. We substitute the Hyperbranch Poly(bismaleimide) as N-Phenylmaleimide containing rich Hyperbranched oligomer to provide the Lithium ion mobility and diffusion rate. It presents less hindrance to Lithium ion transport. Not only can promote the electrochemical performance and safety, but also make the charge-transfer resistance drop down. We bring up a newly method to design a safety additives. To meet the usage of high performance and safety Li-ion batteries.

關鍵字(中)

★ 高分歧
★ 寡聚物

關鍵字(英)

★ hyperbranch
★ oligomer

論文目次

中文摘要……………………………………………………………………….I
英文摘要………………………………………………………………………Ⅱ
目錄……………………………………………………………………………Ⅲ
表目錄…………………………………………………………………………Ⅷ
圖目錄…………………………………………………………………………Ⅸ

第一章緒論……………………………………………………………………1
1-1 前言……………………………………………………………………………………1
1-2 鋰電池原理及組成元件………………………………………………………………2
1-3 鋰電池之關鍵問題……………………………………………………………………2
1-4 研究動機與目的………………………………………………………………………4

第二章文獻回顧……………………………………………………………….9
2-1 鋰電池熱暴升的機制……………………………………………………………….…9
2-1-1 SEI的產生…………………………………………………………………….……9
2-1-2 鹽類及電極的分解………………………………………………………………10
2-1-3 熱爆升機制的鑑定………………………………………………………………10
2-1-4 陰極材料的放熱及氧氣的釋出…………………………………………………13
2-2 安全性改質技術及進展……………………………………………………………15
2-2-1隔離膜……………………………………………………………………………..16
2-2-2阻燃添加劑的機制………………………………………………………………16
2-2-3有機磷系阻燃添加劑……………………………………………………………..18
2-2-4有機氟系阻燃添加劑……………………………………………………………24
2-2-5 SiO添加劑………………………………………………………………………..27
2-2-6過電壓保護添加劑………………………………………………………………29
2-2-7正增溫係數層(PTC)……………………………………………………………30
2-3 常見的安全性研究測試方法……………………………………………………33

第三章高分子電解質………………………………………………………35
3-1 高分子電解質之種類與發展………………………………………………………35
3-1-1 全固態高分子電解質……………………………………………………………35
3-1-2 膠態高分子電解質………………………………………………………………36
3-1-3 孔洞高分子電解質………………………………………………………………37
3-1-4 高分岐狀高分子…………………………………………………………………38
3-1-5 高分岐狀高分子電解質…………………………………………………………42

3-2 Bismaleimide高分歧狀高分子…………………………………………………..……48
3-2-1 Bismaleimide高分歧狀高分子之化學特性……………………………………48
3-2-2 Bismaleimide高分歧狀高分子之結構…………………………………………52
3-2-3 Bismaleimide的熱反應性………………………………………………………56
3-2-4 Bismaleimide/barbituric acid系統………………………………………………57

第四章實驗方法……………………………………………………………61
4-1 實驗藥品……………………………………………………………………………..61
4-2 Hyperbranch bismaleimide的製備方法………………………………………………63
4-3 製備含BMI寡聚物之電解質液………………………………………………………64
4-4 鈕釦型電池組裝……………………………………………………………………64
4-5 1280 mAh方型電池…………………………………………………………………64
4-6 微分掃描熱卡分析儀（DSC）………………………………………………………65
4-7 掃描式電子顯微鏡(SEM)……………………………………………………………65
4-8 熱重分析儀（TGA）分析……………………………………………………………66
4-9 電池性能測試………………………………………………………………………66
4-10 變溫電子自旋共振（VT-ESR）………………………………………………………67
4-10-1基本原理…………………………………………………………………………67
4-10-2外磁場中電子的自旋能級………………………………………………………67
4-10-3 電子自旋共振…………………………………………………………………68
4-11交流阻抗分析 (AC Impedance)……………………………………………………70
4-11-1導電度量測………………………………………………………………………70
4-11-2 等效電路模擬(Equivalent circuit)……………………………………………76
4-12核磁共振光譜(NMR)…………………………………………………………….......78
4-12-1原理簡介…………………………………………………………………………78
4-12-2去氫偶合 (Proton Decoupling)…………………………………………………82
4-12-3魔角旋轉 (Magic Angle Spinning，MAS)……………………………………..83
4-12-4 7Li MAS NMR………………………………………………...………………...84
4-12-5 7Li linewidth theory……………………………………...………………………84
4-12-6脈衝梯度場實驗 (PFR-NMR)………………………………..………………...85
4-13電池安全性測試……………………………………………………………………87

第五章雙酮衍生物的加成聚合之結構及機制……………………………88
5-1 實驗…………………………………………………………………………………89
5-2 反應特性分析………………………………………………………………………89
5-3 寡聚物結構鑑定………………………………………………………………...……94
5-4 雙酮衍生物的加成聚合……………………………………………………………107
5-5 雙酮衍生物的加成聚合之機制……………………………………………………112
5-6 結論…………………………………………………………………………………112

第六章溶劑效應對寡聚物成長的影響……………………………………114
6-1 實驗…………………………………………………………………………………114
6-2 氫光譜分析…………………………………………………………………………115
6-3 雙酮衍生物寡聚物之擴散行為分析………………………………………………121
6-4 結論…………………………………………………………………………………124

第七章鋰離子在BMI高分歧狀寡聚物之動力行為………………………127
7-1 實驗…………………………………………………………………………………128
7-2 高分歧寡聚物之轉化率……………………………………………………………129
7-3 導電度分析…………………………………………………………………………130
7-4 鋰離子動力行為探討………………………………………………………………137
7-5 結論…………………………………………………………………………………142

第八章 BMI高分歧狀寡聚物作為鋰電池添加劑對電性以及安全性的影響
………………………………………………………………………………145
8-1 實驗…………………………………………………………………………………146
8-2 安全特性分析………………………………………………………………………147
8-3 電池性能分析………………………………………………………………………149
8-4 表面形貌分析………………………………………………………………………153
8-5 循環壽命測試………………………………………………………………………158
8-6 電池阻抗組成分析…………………………………………………………………158
8-7 結論…………………………………………………………………………………163

第九章適用於高性能鋰電池的新型高分歧狀寡聚物……………………165
9-1 實驗…………………………………………………………………………………166
9-2 新型寡聚物的合成及鑑定…………………………………………………………168
9-3 表面形貌分析………………………………………………………………………169
9-4 新型寡聚物的導電性及離子動力學分析…………………………………………169
9-5 新型寡聚物的電池性能及阻抗分析………………………………………………176
9-6 新型寡聚物的安全特性……………………………………………………………181
9-7 結論…………………………………………………………………………………182

第十章總結論………………………………………………………………183
參考文獻……...………………………………………………………………185

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指導教授

姚學麟

審核日期

2012-10-23

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