鋰離子二次電池在我們日常生活中扮演了極重要的角色，應用範圍小至手機、平板、筆電的電池大至電動車的電池，都能發現其蹤影，所以如何提升鋰離子電池的儲電量，將成為現今的一大課題；矽作為地殼上僅次於氧含量第二多的元素，擁有無毒性及前處理容易等優點，更重要的是其理論電容量為~4200 mAh/g，相對於市售鋰電池碳負極材料理論電容值372 mAh/g，電量高出十倍，是具有相當優勢的負極材料之一，但在充放電反應時，矽的體積會產生劇烈的膨脹導致顆粒碎裂，造成電容值的急速下降，而此問題將成為矽成為商業化產品的一大阻礙。
本研究將成功地使用不同維度的碳材，分別製備出一維(奈米碳管)、二維(還原氧化石墨烯)和三維(規則中孔洞碳材)的矽-碳複合材料，做為負極材料應用於鋰離子電池上，利用不同種類的碳之結構特性，減緩充放電過程中所帶來體積過度膨脹的問題且避免奈米矽顆粒的聚集，並經由充放電儀測試，得到不同維度下矽-碳複合材料之最佳比例，最後使用其他電化學分析去加以驗證；不同維度：一維、二維及三維之最佳比例的複合材料，經100 mAh/g充放電速率下掃描一百圈下，其電容值分別為~800 mAh/g、~1000 mAh/g及~1300 mAh/g，且庫倫效率皆達到97%以上，表示本研究的複合材料能在長圈數的充放電下，維持材料的結構不受破壞以及電化學反應的穩定性，而未來將可透過此方法，改善在充放電過程中體積膨脹率大的材料上，例如：錫、銻、鎂、鋁等，用以提升鋰離子電池的效能以及增進電容量。

Lithium ion batteries (LIBs) play an important role in our daily life. It has been used for cell phone, ipad, laptop and battery electric vehicle. It is one of the richest topics to improve the battery performance in nowadays. Silicon is present in the earth’s crust at 27.7 % of the total and, after oxygen, is the second most abundant element. In addition, Silicon has been widely used as the anode material for lithium ion batteries (LIBs) because of the huge theoretical capacity (~4200 mAh/g) compared with commercial carbon material (~372 mAh/g) and relatively low discharge potential (~0.5V VS. Li/Li+). However, the large volume expansion (~ 400%) after charge-discharge processes hampers the application of silicon to LIBs.
In this study, we have synthesized successfully that the combination of Si with different dimensional carbon materials including carbon nanotubes (1D), graphenes (2D), and mesoporous carbons (3D) can minimize the volume expansion, resulting in the enhancement of electrochemical performance of silicon-based electrodes. After 100 cycles, the capacity of 1D, 2D and 3D nanocomposites are ~800 mAh/g, ~1000 mAh/g and ~1300 mAh/g respectively. The coulomb efficiency is above 97% remarkably. It shows our different dimensional carbon materials can be maintained structure after charge-discharge and excellent electrochemical stability. In the future, it can provide the method to improve materials which have the large volume expansion after charge-discharge processes, for example Sn, Sb, Mg and Al.

第一章 緒 論 1
1-1 前言 1
1-2 研究動機 3
1-3 研究目的 4
第二章 文獻回顧 5
2-1 鋰離子電池的工作原理 5
2-2 鋰離子電池之內部組件 6
2-2-1 正極材料(Cathode) 7
2-2-2 負極材料(Anode) 11
2-2-3 隔離膜 (Separator) 16
2-2-4 電解液 (Electrolyte) 17
2-3 奈米矽 18
2-4 奈米矽應用於鋰離子電池 20
2-4-1 奈米矽之形貌改變 21
2-4-2 碳基材法 24
第三章 實驗方法與步驟 30
3-1 實驗藥品與器材 30
3-2 實驗架構 32
3-3 一維結構 (Silicon/CNTs) 33
3-4 二維結構 (Silicon/reduced graphene oxide) 34
3-4-1 氧化石墨烯的合成步驟 34
3-4-2 矽與還原氧化石墨烯複合材料之合成 35
3-5 三維結構 (Silicon/ Ordered mesoporous carbons) 36
3-5-1 50 wt% Resol 的合成 36
3-5-2 矽與規則中孔洞碳材複合材料之合成 37
3-6 鋰離子電池之製備與組裝 38
3-6-1 電極材料製備 38
3-6-2 鋰離子電池之組裝 39
3-7 材料特性鑑定及電化學測式 40
3-7-1 X光粉末繞射儀 (X-ray Powder Diffractometer, XRD) 40
3-7-2 比表面積分析儀 (Brunauer-Emmett-Teller specific surface area analyzer, BET) 40
3-7-3 穿透式電子顯微鏡 (Transmission Electron Microscope, TEM) 41
3-7-4 電子能譜儀 (X-ray Photoelectron Spectrometer, XPS) 41
3-7-5 拉曼光譜儀 (Raman Spectroscopy) 42
3-7-6 定電流充放電測試 42
3-7-7 循環伏安法 43
3-7-8 交流阻抗法 43
第四章 結果與討論 44
4-1 不同維度碳材的特性鑑定 44
4-1-1 XRD 44
4-1-2 Raman 46
4-1-3 TEM 48
4-1-4 XPS 49
4-2 不同維度矽-碳複合材料特性鑑定 51
4-2-1 一維矽-碳複合材料：矽與碳奈米管 51
4-2-2 二維矽-碳複合材料：矽與還原氧化石墨烯 56
4-2-3 三維矽-碳複合材料：矽與規則中孔洞碳材 61
4-3 不同維度矽-碳複合材料的電化學表現 66
4-3-1 純矽材料應用於鋰離子電池 66
4-3-2 一維矽-碳複合材料：矽與碳奈米管之電化學表現 69
4-3-3 二維矽-碳複合材料：矽與還原氧化石墨烯之電化學表現 74
4-3-4 三維矽-碳複合材料：矽與規則中孔洞碳材之電化學表現 79
4-4 三種不同維度結構的複合材料之間長圈數下的電化學表現 83
第五章 結 論 88
5-1 不同維度矽-碳複合材料之合成 88
5-2 不同含矽比例的複合材料特性探討與其電化學行為 88
5-3 不同維度最佳化比例在充放電長圈數下的電化學行為 89

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