隨著科技的發展，人們對於二次儲能元件的需求與日俱增，其中鋰離子電池因具有高能量密度以及較大的工作電壓而備受關注，但其功率密度與循環壽命仍有很大的改善空間。鋰離子電容器結合了鋰離子電池與超級電容器之電極，在維持一定能量密度下提高功率密度與循環壽命，是近幾年較為新穎之儲能裝置。為了發展出性能更優異的鋰離子電池/電容器，各式各樣的材料被提出並檢測其應用潛力，其中，矽因擁有最高的理論比電容值(3579 mAh g-1)而受到許多矚目，較低的嵌鋰電位使電池能擁有較大的工作電壓，在地殼中豐富的儲量也使矽之取得價格相對低廉。然而，矽材在充放電過程中劇烈的體積變化(300 %)使其容易從集電板上脫落，導致循環壽命與穩定性低落而限制了發展空間。
為了改善此現象，本研究以一鍋(one pot)法合成以RF樹脂(Resorcinol-Formaldehyde resin)包覆之二氧化矽奈米球(SiO2@RF)，在經過碳化及鎂熱還原後，得到具有core-shell結構的矽碳複合材料(Si@RFC)。藉由調整前驅物添加比例以及反應時的溶液組成比例(Ethanol/Water ratio, E/W)，分別調控不同的RF樹脂厚度以及產物粒徑大小，有效地抑制副產物碳化矽產生，調控產物之成分組成，得到具有最高放電比電容值之Si@1RFC (E/W=2)。透過硼元素摻雜以及添加還原氧化石墨烯(reduced Graphene Oxide, rGO)，B-Si@1RFC/rGO，進一步提升比電容值、導電度與循環穩定性，在三者的偕同效應下而具有良好的電化學表現。
本研究亦採用水熱法與化學活化法，製備葡萄糖衍生奈米碳球(Glucose derived Carbon NanoSphere, GCNS)，具有超高比表面積(1947 m2 g-1)，與極佳的循環穩定性。B-Si@1RFC/rGO//GCNS鋰離子電容器結合兩材料優點，於2.0~4.5 V (vs. Li/Li+)的電位區間，在0.328 kW kg-1功率密度下達到149 Wh kg-1的能量密度，而在49.3 kW kg-1之高功率密度下仍保有82.1 Wh kg-1的能量密度。且在5 A g-1電流密度下經過20,000圈充放電，仍有67.3 %的電容維持率，兼具高能量、高功率密度，以及優異的循環穩定性。

With the growing demands for sustainable energies in response to the application in electric vehicles and portable electronic devices, research and development in energy storage devices becomes increasingly more critical. Lithium ion batteries (LIBs) continue to draw intensive and extensive research attention because of their high energy densities and working voltages. However, low power densities and unsatisfactory cycling life limit their further applications. To overcome this obstacle, lithium ion capacitors (LICs), which combine the advantages of lithium ion batteries and supercapacitors, were developed and demonstrated high power densities when maintaining decent energy densities. A wide range of materials have been investigated as potential electrode materials for LIBs and LICs. Among them, silicon captures much research attention because of its ultrahigh theoretical specific capacity (3579 mAh g-1). However, the drastic volume expansion (~300 %) induced by lithiation causes the loss of contact between the active material and the current collector, resulting in poor stability and cycling life of the battery.
In this work, we developed a one pot synthetic method to prepare core-shell SiO2-RF composites (SiO2@RF) through simultaneous condensation of resorcinol-formaldehyde resins and sol-gel reaction of tetraethoxysilane (TEOS). The as-synthesized SiO2@RF was converted into core-shell Si@RFC through carbonization followed by magnesiothermic reduction. By adjusting the ratio of the precursor of silica versus resin and the ratio of ethanol versus DI water used in the synthesis, the product composition and particle size could be manipulated, respectively. Product B-Si@1RFC/rGO combines the benefits of high specific capacities of Si@1RFC, enhanced electronic conductivities of boron doped Si, and good stability of rGO, and hence exhibits excellent electrochemical performances because of the corresponding synergistic effect.
Glucose derived carbon nanospheres (GCNS) were synthesized with a hydrothermal method followed by chemical activation to serve as the cathode materials. GCNS shows high specific surface area of 1947 m2 g-1 and excellent cycling stability. B-Si@1RFC/rGO//GCNS LIC combines the merits of Si@1RFC/rGO and GCNS, demonstrating a high energy density of 149 Wh kg-1 at a power density of 0.328 kW kg-1, and maintains a decent energy density of 82.1 Wh kg-1 at a high power density of 49.3 kW kg-1. The LIC also shows good cycling stability at a current density of 5 A g-1, exhibiting a 67.3 % capacity retention after a 20,000 cycle operation.

摘要 ………………………………………………………………………………… i
圖目錄 ……………………………………………………………………………ix
表目錄 ……………………………………………………………………………xiv
第 1 章 緒論 1
1-1 前言 1
1-2 鋰離子電池 2
1-3 超級電容器 4
1-4 鋰離子電容器 6
1-5 One pot法合成簡介 7
第 2 章 文獻回顧 8
2-1 概述 8
2-2 中空奈米球結構 9
2-3 異原子摻雜 14
2-4 以RF樹脂包覆之二氧化矽應用 17
2-5 以rGO導電網絡包覆之雙碳層中空矽球 18
2-5 實驗動機 20
第 3 章 實驗方法與儀器 22
3-1 實驗藥品 22
3-2 實驗器材 26
3-3 分析儀器 27
3-4 實驗流程 29
3-4-1製備以RF樹脂包覆之二氧化矽奈米球 29
3-4-2 碳化及鎂熱還原 31
3-4-3 硼元素摻雜 32
3-4-4以還原氧化石墨烯包覆硼摻雜矽碳複合物 32
3-4-5葡萄糖衍生碳材製備 33
3-4-6不鏽鋼網集電板前處理 34
3-4-7極片製備及陰陽極半電池組裝 34
3-4-8陰陽極活性物質配重及鋰離子電容器組裝 35
3-4-9 電化學分析 35
第 4 章 結果與討論 38
4-1 TEOS與RF比例之影響 (E/W=7) 38
4-1-1 SiO2@xRFC奈米球 38
4-1-2 Si@xRFC奈米球 41
4-1-3 電化學分析 44
4-2 溶劑組成比例之影響 48
4-2-1 SiO2@1RFC奈米球 48
4-2-2 Si@1RFC奈米球 52
4-2-3 電化學分析 54
4-3 TEOS與RF比例之影響 (E/W=2) 55
4-3-1 SiO2@xRFC奈米球 55
4-3-2 Si@xRFC奈米球 58
4-3-3 電化學分析 60
4-4 硼摻雜之影響 62
4-4-1 材料分析 62
4-4-2 電化學分析 66
4-5 添加rGO之影響 67
4-5-1 rGO之材料與電化學分析 68
4-5-2 rGO添加比例之影響 70
4-6 GCNS之材料與電化學分析 73
4-7 鋰離子電容器 77
第 5 章 結論 82
參考文獻 83

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