鋰離子電容器為一種新穎的儲能裝置，其結合了鋰離子電池及超級電容器的優點，在保有高能量密度的同時，又能擁有高功率密度。其中，鋰離子電容器的陽極材料為一個很有發展潛力的方向，由於現今商業化使用的石墨理論容量值較低（372 mAh g-1），不足以應付未來需求。目前眾多研究致力於開發其它具有潛力的陽極材料，例如金屬氧化物、矽材及複合材料等，其中，三氧化二鐵(Fe2O3)在金屬氧化物中具有相對較高的理論比容量（1007 mAh g-1），且其成本低廉和無毒的特性，被認為是鋰離子電容器最具潛力的陽極材料之一。
三氧化二鐵雖擁有諸多優點，但普遍上仍有許多不可忽視的困難存在，例如倍率性較差及容量衰退等，造成三氧化二鐵在實際應用上的限制。而中空多孔的奈米結構可以有效的改善上述問題，在高電流密度下，其中空多孔結構能有效促進鋰離子的傳輸，以改善其倍率性，另外，此結構能提供體積膨脹收縮緩衝的空間，使奈米結構不易因此瓦解，以改善容量衰退的問題。因此，本研究致力於合成中空多孔結構的三氧化二鐵，成功地使用一步驟溶劑熱法製備出中空多孔三氧化二鐵(α-Fe2O3 hollow porous nanoparticles, α-Fe2O3 HPNPs)，其比表面積達到67m2 g-1，並且具有充足的微孔及介孔，本研究將其進一步應用做為鋰離子電容器之陽極。
在鋰離子電容器之陽極半電池中，α-Fe2O3 HPNPs有非常優異的電化學表現，在0.2 A g-1的電流密度下，達到1103 mAh g-1的高比電容值，且在4 A g-1的高電流密度下還保有822 mAh g-1的比電容值，展現出極佳的倍率性。在0.2 A g-1下循環200圈後，由於活化現象而達到1341 mAh g-1的高比電容值。在鋰離子電容器中，本研究將α-Fe2O3 HPNPs作為陽極、葡萄糖衍生之奈米碳球 (Glucose derived Carbon Nanospheres, GCNS)作為陰極，組裝成鋰離子電容器，其在0.24 kW kg-1的功率密度下展現出 107 Wh kg-1的高能量密度，且在9.68 kW kg-1的高功率密度下還能保有 86 Wh kg-1的能量密度，展現相當優異的倍率性。此外，在1 A g-1下循環2500圈後仍擁有84%的電容維持率。α-Fe2O3 HPNPs之優異電化學表現可以歸因於其中空多孔結構，如同奈米電化學反應器，其內部空間能有效使鋰離子擴散路徑縮短，並且提供體積膨脹收縮的緩衝空間，使其擁有優秀的倍率性及循環長效性。

As a novel energy storage device, lithium ion capacitors (LICs) integrate the merits of both lithium ion batteries (LIBs) and supercapacitors (SCs). Because of this unique feature, LICs possess high energy densities without sacrificing power densities. The most commonly used anode material in commercial LIBs is graphite, and because of the energy storage mechanism, its theoretical specific capacity is only 372 mAh g-1, which does not meet the demand of future energy storage devices. It is thus critical to develop alternative anode materials, such as metal oxides, silicon, and composites. Compared to other metal oxides, Fe2O3 possesses a relatively high theoretical specific capacity (1007 mAh g-1), together with its low cost and non-toxic nature, making it one of the most promising anode materials for lithium ion based energy storage.
Nevertheless, there are still issues to be resolved for commercialization of Fe2O3 anodes. Most notably, its poor rate capability and rapid decay in capacity at cycling limit its practical applications. It is proposed that nano-sized hollow porous structure can effectively address the issues. When operating at high current densities, the hollow porous structure serves as nanoreactors to enable local fast charging/discharging, leading to improved rate capability. Moreover, the void of the hollow structure also serves as buffer space to accommodate the volume expansion and shrinkage during the charge and discharge cycle, preventing the collapse of the structure and thus improving the cycling performance. In this work, we report the synthesis of hollow porous α-Fe2O3 nanoparticles (α-Fe2O3 HPNPs) with a one-step solvothermal process. The surface area of α-Fe2O3 HPNPs is determined to be 67m2 g-1, possessing abundant micro- and meso-pores. The as-synthesized α-Fe2O3 HPNPs are applied as the anode material for assembly of LICs.
When tested as an anode half-cell, α-Fe2O3 HPNPs exhibit high specific capacities of 1103 and 822 mAh g-1 at current densities of 0.2 and 4 A g-1, respectively, indicating its excellent rate capability. After 200 cycle operations at 0.2 A g-1, the specific capacity increases to 1341 mAh g-1 because of the accompanying electrochemical activation. This α-Fe2O3 HPNPs anode is further paired with a glucose derived carbon nanospheres (GCNS) cathode to form an LIC. The α-Fe2O3 HPNPs//GCNS LIC delivers a high energy density of 107 Wh kg-1 at the power density of 0.24 kW kg-1 and maintains a satisfactory energy density of 86 Wh kg-1 at a high power density of 9.68 kW kg-1, revealing its excellent rate capability. Furthermore, a high capacity retention rate of 84 % is achieved after 2,500 cycle operations at 1 A g-1, showing an outstanding cycling performance. The excellent electrochemical performance of α-Fe2O3 HPNPs can be attributed to its unique advantageous structure, with the inner void acting as a nano-reservoir of electrolyte to shorten the diffusion path of lithium ions and serving as buffer space to accommodate the large volume variation during cycling.

摘要 I
圖目錄 VIII
第1章 緒論 1
1-1 前言 1
1-2 二次儲能元件 2
1-2-1 概述 2
1-2-2 鋰離子電池簡介 3
1-2-3 超級電容器簡介 6
1-2-4 鋰離子電容器簡介 8
1-3 三氧化二鐵 9
1-3-1 概述 9
1-3-2 三氧化二鐵之儲鋰機制 10
1-4 研究動機 12
第2章 文獻回顧 13
2-1 概述 13
2-2 以鋰離子為基礎的能量儲存陽極材料 13
2-2-1 碳材 13
2-2-2 過渡金屬氧化物 14
2-2-3 矽材 15
2-3 中空多孔金屬氧化物於以鋰離子為基礎的能量儲存陽極材料 17
第3章 實驗方法與儀器 24
3-1 實驗藥品 24
3-2 實驗器材 25
3-3 分析儀器 26
3-4 實驗流程 29
3-4-1 α-Fe2O3 HPNPs之製備 29
3-4-2 葡萄糖衍生之奈米碳球製備 31
3-4-3 陽極半電池製備 31
3-4-4 陰極半電池製備 32
3-4-5 鋰離子全電池組裝 32
3-4-6 電化學分析實驗 33
第4章 結果與討論 35
4-1 溶劑熱反應過程產物分析 35
4-2 中空多空結構之材料分析 43
4-3 電化學分析 47
4-3-1 中空多孔三氧化二鐵之陽極半電池分析 47
4-3-2 葡萄糖衍生之碳奈米球GCNS之陰極半電池分析 58
4-3-3 鋰離子電容器分析應用 59
第5章 結論 68
參考文獻 70

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