臺灣博碩士論文加值系統

本研究是利用中國碳素鋼鐵公司提供之活性碳做為超高電容器的電極，並調控不同持溫的溫度、不同熱處理氣氛以及活性碳本身顆粒大小；藉以探討活性碳表面官能基和活性碳顆粒大小對超高電容器性質的影響，而其中電解液是選用商業上較常運用的1 M TEABF4/PC (Tetraethylammonium Tetrafluoroborate)/(Propylene Carbonate)做為電解液。
首先探討不同熱處理溫度對電容器的影響：本實驗在450 oC、600 oC、750 oC、850 oC、950 oC氮氣下進行熱處理，由材料分析能夠觀察到：隨著熱處理溫度提高，除了降低活性碳比表面積外、其表面含氧官能基含量也隨之下降；在電化學分析方面，提高溫度江造成的比表面積減少，其結果反應在低速電容值的下降；然而表面含氧官能基含量的減少能增進電容器的耐用度(循環穩定性、高速穩定性、漏電流特性等)。
根據上述實驗結果，進一步討論在750 oC下不同氣氛下進行熱處理對電容器的影響；比較N2、NO、NH3、Melamine等氣氛，預期透過氮摻雜提高電容器的性能。由材料分析中能發現：使用不同熱處理方式皆能有效的對碳材進行摻氮，其中以Melamine所摻雜之氮含量最多；電化學分析方面，顯現NO熱處理方式在穩定性上有較佳的表現。
另一方面，將不同粒徑分布的活性碳透過750 oC氮氣熱處理，試觀察不同粒徑尺寸對於超高電容器性質的影響。在材料分析中能夠得知：隨著粒徑尺寸越小，其碳材表面所含氧官能基的量也越多，進而影響電容器的電化學性質(循環穩定性、高速穩定性、漏電流特性等)。

In the present study, the activated carbon obtained from China Carbon Steel Company was used as the electrode for the super capacitor. The different heat treatment temperature, atmosphere, and the particle size of activated carbon were controlled and their effects were studied comprehensively to understand the electrochemical behavior of super capacitor. 1M TEABF4 (Tetraethylammonium Tetrafluoroborate)/PC (Propylene) was used as an electrolyte. The effects of different heat treatment temperatures (450, 600, 750, 850 and 950 °C) on the capacitors were investigated. This study shows that with increasing the heat treatment temperature, the oxygen content on the surface of activated carbon and the specific surface area reduced leading to decrease in the capacitance at low-current density. However, the decrease in the content of the oxygen-containing functional groups can improve the durability of the capacitor (cycle stability, high-rate performance, leakage current characteristics, etc.). On the basis of the above experimental results, the effects of heat treatment on the capacitors were investigated under different atmospheres at 750°C. Also, we doped Nitrogen in the activated carbon by using different heat treatment atmosphere (Melamine, NO, and NH3) to improve the performance of the capacitors.
Further, the activated carbon with different particle size distribution was heat treated at 750 °C in the nitrogen atmosphere. The effect of particle size on the properties of super capacitor was investigated. It is found that the smaller the particle size, the more the amount of oxygen functional groups is contained on the surface of the carbonaceous material and as result of which affects the electrochemical properties of the capacitor (cycle stability, high-speed stability, leakage current characteristics, etc.).

摘要 I
Abstract III
誌謝 V
總目錄 VII
表目錄 IX
圖目錄 XI
第一章 緒論 1
1-1 前言 1
1-2 研究動機 1
第二章 研究背景與文獻回顧 2
2-1 超高電容器簡介 2
2-2 影響電雙層電容器電容值的因素 4
2-3 含氧官能基影響 6
2-3-1 含氧官能基產生原因 6
2-3-2 含氧官能基對電容產生之負面影響 7
2-3-3 熱處理移除含氧官能基 8
2-3-4 運用熱處理進行活性碳移除含氧官能基對超級電容電化學之影響 9
2-4 摻氮官能基 15
2-4-1 摻氮原因 15
2-4-2 摻氮方法 16
2-4-3 不同氣氛下摻雜氮原子 16
2-4-4 對活性碳材進行摻氮探討其對電化學行為之影響 18
2-5 活性碳粒徑大小 26
2-5-1 活性碳顆粒大小造成之影響 26
2-5-2 活性碳顆粒大小於超級電容中之應用 27
第三章 實驗方法與步驟 32
3-1 活性碳材料取得 32
3-2 材料特性鑑定 32
3-2-1 碳材形貌之分析 32
3-2-2 碳材官能基鑑定 32
3-2-3 活性碳比表面積量測 33
3-3 電化學測試實驗步驟 34
3-3-1 循環伏安法(Cyclic Voltammetry，CV) 35
3-3-2 計時電位法 (Chronopotentimetry，CP) 36
3-3-3 交流阻抗(Electrochemical Impedance Spectroscopy，EIS) 36
3-3-4 漏電流測試(Leakage Current) 36
3-3-5 循環穩定性分析(Cycle Life Test) 37
3-3-6 氣脹分析 37
第四章 結果與討論 38
4-1 活性碳材於不同熱處理溫度比較 38
4-1-1 材料結構分析 38
4-1-2 官能基鑑定 40
4-1-3 電化學性質 43
4-1-4 高壓方面之電化學性質 51
4-2 活性碳材於不同黏著劑之電化學性能比較 59
4-2-1 電化學性質 60
4-3 活性碳材於不同熱處理進行摻氮比較 66
4-3-1 材料結構分析 66
4-3-2 官能基鑑定 69
4-3-3 電化學性質 74
4-4 不同粒徑活性碳材對於電化學之影響 85
4-4-1 材料結構分析 85
4-4-2 官能基鑑定 91
4-4-3 電化學性質 96
第五章 結論 106
活性碳材於不同熱處理溫度比較 106
活性碳材於不同黏著劑比較 106
活性碳材於不同摻氮方法比較 106
活性碳材於不同粒徑大小比較 107

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