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研究生：	曾宇呈 Tseng, Yu-Cheng
論文名稱：	鋰離子電容負極碳材結構對儲能之影響 Influence of Carbon Anode Structure on the Performance of Lithium-Ion Capacitors
指導教授：	鄧熙聖 Teng, Hsisheng
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 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：	112
中文關鍵詞：	鋰離子電容器、石墨、軟碳、硬碳、嵌鋰阻抗
外文關鍵詞：	lithium-ion capacitors, graphite, soft carbon, hard carbon, Li+ insertion resistance
相關次數：	點閱：50 下載：0
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鋰離子電容(lithium-ion Capacitors, LICs)為結合電雙層電容(Electric double-layer Capacitors, EDLCs)與鋰離子電池(lithium-ion Batteries, LIBs)兩者優點的儲能裝置，其正極為具高比表面積之活性碳，負極分別為鋰化後之石墨、軟碳、硬碳，三種碳材料。LICs具有較EDLCs高的能量密度，功率密度較LIBs高，但仍稍低於ELDCs。本研究中探討上述三種不同負極碳材料之石墨烯層堆疊規律性、結晶度、d-spacing等材料結構對於鋰離子電容儲能效果之影響。而預鋰化後的硬碳負極，與中鋼碳素活性碳正極(ACS系列)搭配1M LiPF6 @EC+DMC電解液製備成鋰離子電容後具有較優良之效能。由於硬碳在結構上具有部分石墨微晶區及部分排列不規則區，且硬碳具有較大的層間距(d spacing)，使其在快速充放電時相較於其他的負極材料有較高的電容維持率。由於硬碳此種特殊的結構，使鋰離子在硬碳結構中進行嵌入/嵌出時的阻抗較小。HC-LIC在操作電位2-4 V下，以0.5 A g-1的電流進行2000圈循環壽命測試可保持約96%之電容維持率，此外，HC-LIC以1 A g-1的電流進行10000圈循環壽命測試亦可保持約81%之電容維持率，顯示硬碳負極在高充放電速率下進行長效測試之穩定性，而HC-LIC的能量密度(95 Wh kg-1)與功率密度(13 kW kg-1)亦優於其他文獻，展現硬碳應用於鋰離子電容的優異性。本研究結果指出使用直接接觸預鋰化法搭配具有部分非結晶區及較大的層間距的負極材料，可提升鋰離子電容在快速充放電以及具有較優異的循環壽命表現。

By combining the energy storage features of electric double-layer capacitors (EDLCs) and lithium-ion batteries (LIBs), lithium-ion capacitors (LICs) have been studied widely as a novel energy storage device with high energy density, large power density and excellent cycling stability. Recently, many different kinds of carbon materials have been introduced as the electrode material of LICs due to cheap cost, environment friendly and superior electrochemical stability. In this work, we combine AC cathode with three different structure carbon materials, that is graphite (GR), soft carbon (SC), and hard carbon (HC), as anode to assemble LICs. These anode materials with different structure effect show different Li+ insertion resistance, and thus influence the electrochemical performance of LICs. Among all LICs in this work, HC-LIC shows the best high rate performance (53% at 7 A g-1) and cycling performance (81% after 10k cycle). HC-LIC also shows higher energy density (95 Wh kg-1) and power density (13 kW kg-1) comparing to others literature.

中文摘要	I
英文延伸摘要	II
致謝	IX
總目錄	XII
表目錄	XVI
圖目錄	XVII
第一章 緒論	1
1-1 前言	1
1-2 超級電容器的發展與應用	3
1-3超級電容器元件構造介紹	7
1-3-1電極材料	8
1-3-2電解質	10
1-3-3集電器	12
1-3-4黏著劑	12
1-3-5隔離膜	13
1-4 超級電容器之儲能機制	14
1-4-1電雙層電容器	14
1-4-2 擬電容	15
1-4-3 混合型電容器	16
1-5 研究動機	17
第二章 文獻回顧與理論說明	18
2-1 電雙層結構與原理	18
2-1-1 電雙層原理	18
2-1-2 Helmholtz 電雙層模型	18
2-1-3 Stern 電雙層模型	19
2-1-4 電容器簡介	21
2-1-5 兩極式與三級式電容器	22
2-2 碳材孔隙分析原理	23
2-2-1 等溫吸附曲線	23
2-2-2 BET 等溫吸附模式	27
2-2-3 BJH理論	28
2-2-4 密度泛函理論(Density Functional Theory, DFT)	28
2-3鋰離子電容(Lithium-Ion Capacitors, LICs)	32
2-3-1鋰離子電容儲能機制	34
2-3-2鋰離子電容正極材料	36
2-3-2-1碳材料	36
2-3-2-2鋰氧化物複合材料	37
2-3-3鋰離子電容負極材料	38
2-3-3-1 碳材料	39
2-3-3-2 非碳材料	40
2-3-4預鋰化(Prelithiation)	42
2-3-4-1電化學預鋰化法(Electrochemical Prelithiation)	42
2-3-4-2直接接觸預鋰化法(Direct Contact Prelithiation)	43
2-3-4-3 含鋰活性物質預鋰化	45
2-4 電雙層電容器與鋰離子電容器之比較	47
2-5 電化學測試原理	48
2-5-1 循環伏安法	48
2-5-2 定電流充放電	49
2-5-3 電化學阻抗頻譜分析	51
第三章 實驗方法與儀器原理介紹	56
3-1 藥品、材料與儀器設備	56
3-1-1 實驗用藥品與材料	56
3-1-2 儀器與實驗設備	57
3-2 實驗步驟	58
3-2-1 極片製備	58
3-2-1-1 活性碳正極極片製備	58
3-2-1-2 負極極片製備	58
3-2-2 鈕扣型鋰離子電容負極half cell組裝	59
3-2-3 直接接觸預鋰化法	60
3-2-4 軟包型鋰離子電容組裝	60
3-3 電化學分析	61
3-3-1 循環伏安法測試	61
3-3-2 定電流充放電測試	61
3-3-3 長效循環壽命測試	61
3-3-4 電化學阻抗頻譜分析	62
3-4 儀器分析原理簡介	63
3-4-1氮氣物理吸脫附分析	63
3-4-2 穿透式電子顯微鏡 (Transmission Electron Microscope, TEM)	65
3-4-3 X光繞射分析 (X-ray Diffraction, XRD)	67
3-4-4 掃描式電子顯微鏡(Scanning Electron Microscope, SEM)	69
第四章 結果與討論	72
4-1 三種負極材料之特性分析	72
4-1-1 三種負極材料比表面積與孔徑分布分析	72
4-1-2 TEM結果探討	74
4-1-3 X-ray繞射圖譜分析	76
4-2 三種負極材料電化學分析與預鋰化負極表面分析	77
4-2-1 負極材料半電池循環伏安測試	77
4-2-2 預鋰化SEM分析	79
4-3 三種負極材料應用於鋰離子電容之電化學測試	81
4-3-1 三極式開環電位測試	81
4-3-2 循環伏安法分析	83
4-3-3 定電流充放電測試	85
4-3-4 鋰離子電容器交流阻抗分析	89
4-3-5 鋰離子電容器電化學性能比較	92
4-4 文獻比較	99
第五章 結論	102
參考資料	104

                                    

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