臺灣博碩士論文加值系統

超級電容器是近幾十年發展出的一種新型儲能元件，和一般電容器的差異在於具備高能量密度、快速充放電速率以及使用壽命長的特性。由於能源危機以及環保意識的逐漸抬頭，利用人類垃圾資源回收再利用來製備活性碳作為儲能材料之原料，除了可以解決地球資源匱乏問題之外，也能達到綠色環保、節能減碳的訴求。在超級電容中，製備高孔隙率的活性碳是一個必備的條件，而活化劑在這過程中就扮演了一個重要的角色，因為較大的比表面積可以增加電極和電解液的接觸面積，使得超級電容的效能增加。因此活化劑對於製備活性碳之物理性質以及其電化學的表現行為是建立高效能活性物質一個值得探討的議題。
本篇論文是使用回收的香菸濾嘴 (CF) 通過管狀爐高溫預碳化和利用不同酸鹼性的化學藥品如氫氧化鉀、磷酸、氯化鋅當作活化劑的化學活化法製成活性碳，以作為超級電容的活性碳儲能材料，然後使用聚偏二氟乙烯 (PVDF) 做為黏著劑，將活性碳塗佈於碳布上作為電極，研究結果顯示使用由氫氧化鉀製成的活性碳 (CAC-KOH) 電極在電流密度為 0.5 A/g 下可達到 106.5 F/g 的最大比電容值，是市售活性碳電極的 2.1倍 (50.0 F/g)，接著我們使用最佳表現之活性碳電極組成對稱型超級電容器，其於電流密度 0.5 A/g 量測下可達到 1.3 V 的電位窗及 21.9 F/g 的比電容值。在功率密度為 325 W/kg 時，此對稱型超級電容器達 5.15 Wh/kg 的能量密度。另外，電極在進行 11000 次重複循環充放電過程後，此對稱型超級電容器可達到 73% 的電容保留率及 88% 的庫倫效率。未來期盼可以使用更多的垃圾資源回收材料利用活化劑的處理程序來製備活性碳成為高性能的電極材料，以達到低成本及環境友善的綠色儲能裝置。

The Supercapacitor is a new type element of energy storage capability developed in recent decades. It has different general capacitors due to its excellent properties of higher power density, faster charge-discharging rate and longer cycle life. Due to the energy crisis and the gradual rise of environmental awareness, using raw materials produced from the wastes and biomasses to synthesize activated carbon can not only solve the resource scarcity problem but also meet the demands of green environmental protection, energy saving and carbon reduction. High porosity is the prerequisites condition to prepare activated carbon in supercapacitors, and the activator plays an important role in this process. The effectiveness of the supercapacitor is increased because a larger specific surface area can increase the contact area between the electrode and the electrolyte. Therefore, the effects on the physical properties and electrochemical behavior of the activating agent for the preparation of activated carbon are worthy to investigate.
In this thesis, we used the waste cigarette filters (CF) to produce activated carbon through the high temperature carbonization and chemical activation method of the tubular furnace, which is used as the activated carbon energy storage material of the supercapacitor. Three kinds of alkaline, acid and neutral activating agents including potassium hydroxide (KOH), Phosphoric acid (H3PO4) and zinc chloride (ZnCl2) were applied to activate the waste cigarette filters for producing activated carbon. Subsequently, the activated carbon electrode was fabricated by using the carbon cloth substrate and the binder polyvinylidene fluoride (PVDF). The KOH-activated carbon electrode shows the highest specific capacitance of 106.5 F/g, which is two-fold of that for the commercial activated carbon electrode (50.0 F/g), The symmetric supercapacitors with the KOH-activated carbon (CAC-KOH) electrodes at the potential window of 1.3 V shows a specific capacitance of 21.9 F/g, and the maximum energy density of 5.15 Wh/kg at the power density of 325 W/kg. The specific capacitance retention of 73% and Coulombic efficiency of 88% during the 11000 times charging/discharging process were also obtained. In the future, other more waste recycling materials can be used to prepare activated carbon by using the efficient activating agent process to become high-performance electrode materials and achieve the low-cost and environmentally friendly green energy storage devices.

摘 要………i
ABSTRACT………iii
致 謝………v
目錄………………………vi
表目錄…………………ix
圖目錄……………………x
第一章 緒論……1
1.1 前言……1
1.2 研究動機 ………3
第二章 文獻回顧 ………4
2.1 超級電容器…4
2.1.1 簡介…………………4
2.1.2 儲能機制…………6
2.1.2.1電雙層電容器…………6
2.1.2.2擬電容電容器…………7
2.1.2.3混合型電容器…………8
2.1.3 組裝結構……………………………………………9
2.1.3.1對稱型超級電容器………………9
2.1.3.2非對稱型超級電容器…………9
2.2 超級電容器元件…………………………………………10
2.2.1 導電基材……………………………………………………………10
2.2.2 電解液種類………………………………………………………11
2.2.2.1水溶液電解液……………………11
2.2.2.2有機電解液…………………………11
2.2.2.3離子液體電解液………………11
2.2.2.4半固態電解液……………………12
2.2.3 儲能材料…………………………………………………………12
2.2.3.1金屬化合物……………………………12
2.2.3.2導電高分子……………………………13
2.2.3.3碳材……………………………………………13
2.3 資源回收活性碳………………………………………16
2.3.1簡介…………………………………………………16
2.3.2製造方法…………………………………………………………18
2.3.2.1前處理……………………………………18
2.3.2.2碳化…………………………………………18
2.3.2.3活化…………………………………………18
2.3.2.4後處理……………………………………20
2.3.3應用……………………………………………………………………20
第三章 藥品儀器與實驗方法……………………………24
3.1 實驗藥品…………………………………………………………24
3.2 實驗儀器……………………………………………………………25
3.2.1製程儀器………………………………………25
3.2.2物性分析儀器……………………………26
3.2.3電化學分析儀器………………………27
3.3 實驗流程……………………………………………………………28
3.3.1碳布基材………………………………………28
3.3.2香菸濾嘴前處理………………………28
3.3.3製備香菸濾嘴活性碳……………29
3.3.4電極製備……………………………………30
第四章 物性與電化學分析原理………31
4.1 掃描式電子顯微鏡 (Scanning electron microscope, SEM)……31
4.2 X 射線繞射儀 (X-ray diffractometer, XRD) ………………32
4.3 傅立葉轉換紅外光譜儀 (Fourier-transform infrared spectroscopy, FTIR)…33
4.4 比表面積與孔隙分佈分析儀 (Specific surface area & pore size distribution
analyzer by gas adsorption method)………………34
4.5 拉曼光譜儀 (Raman spectroscopy)……36
4.6 接觸角測量儀(Contact angle meter…37
4.7 循環伏安法 (Cyclic voltammetry, CV)………………38
4.8 恆電流充放電 (Galvanostatic charge-discharge, GC/D)………………39
4.9 電化學阻抗圖譜 (Electrochemical impedance spectroscopy, EIS)………………40
第五章 結果與討論………………41
5.1 物性分析………………41
5.1.1 不同活化劑製備之活性碳結構分析………………41
5.1.2 不同活化劑製備之活性碳組成分析………………42
5.2 三極式電化學分析………………49
5.2.1 不同活化劑製備之活性碳電化學量測分析………………49
5.2.2 不同掃描速率與電流密度量測分析………………51
5.2.3 市售活性碳與香菸濾嘴製備活性碳之電極電化學表現比較………53
5.2.4 降低活化溫度電化學量測分析………………56
5.3 對稱型電容器電化學分析………………57
第六章 結論與建議………………60
6.1 結論………………60
6.2 建議………………61
參考文獻………………62

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