軟碳材料過去曾被利用於鋰離子電池系統，其原因為高速率充放電能力比石墨好，在快速充放電速率下，電容值較高，近年來軟碳漸漸開始應用在快速充放電系統，如鋰離子電容器；因此，如將此特性應用於有機相高電壓超高電容器，就有機會提高其能量密度，彌補超級電容器低能量密度的缺點，是一項新穎且具有競爭力的領域。
本研究首先專注在評估純軟碳之石墨結晶大小與孔洞性等，對其應用於有機系之超高電容的電化學行為影響。其二，根據前述軟碳微結構之差異，對於有機電解質之陰離子的嵌入/嵌出的速率與電容量之影響，做一釐清。
因欲達到更高的電容量，本研究針對軟碳進行KOH活化。利用KOH化學活化，將軟碳蝕刻出微孔或甚至潛孔結構，以增加比電容、可逆性、高速充放電之電化學性能。實驗結果顯示，經過KOH活化後的軟碳具有能夠電化學活化的特性，利用第一圈充放電建立離子可以吸/脫附或嵌入/嵌出的活性位置，並展現良好的電雙層電容行為。
值得注意的是，經過KOH活化後的軟碳比表面積仍然很低，且密度高，屬於無孔結構，經過電化學活化，其電容值劇烈地提高，儲能特性有如傳統電雙層電容，其材料特性與傳統活性碳(高比表面積)特徵不同，且因比表面積較低，碳材表面不易吸附水氣，故正極上限工作電位窗至少可達2V。研究結果為，鹼活化軟碳SA03當正極電位窗2.6 V (-0.6V – 2.0V) 時，比電容可達65 F/g。
因KOH活化的效果與軟碳微結構多寡有直接關係，因此，利用實驗設計法找到最佳的KOH活化參數組合，及電化學活化參數是需要的，由實驗設計結果得知，選擇SA04軟碳、碳與KOH混合比例為1:5、KOH活化溫度為720℃及電化學活化電位越高，能夠得到最大電容值，但如果要考慮庫倫效率，上限電位必須修正為1.4V，目前研究結果，由最佳參數製作出的鹼活化軟碳，正極電位窗為2.0V時(-0.6V – 1.4V)，重量比電容為100 F g-1，體積比電容為65 F cm-3。
為了組成非對稱式超高電容，將鹼活化SA04軟碳當作正極，商用活性碳ACS25當作負極，得到全電池電壓3.8V，若根據兩極活性材料重量，電容為30 F g-1，庫倫效率95 %，能量密度58.16 Wh kg-1，功率密度1.85 kW kg-1。

In the first part, this essay aims to debate the influences of graphite domain size, graphite microcrystalline degree and pore microstructures on the capacitive behavior of soft carbons through electrochemical analyses and material characterizations. The relationship between charge capacity of soft carbon and quantities of anions intercalation/de-intercalation is established to clarify the charge storage mechanism. From the results of electrochemical analysis and XRD, there is a positive correlation between electrochemical activation and d-spacing of graphene layers. When the soft carbon has larger d-spacing, the percentage of capacitance increase after the electrochemical activation is higher. Furthermore, the absolute value of capacitance is greater if the soft carbon has more graphite-like microcrystalline structures along the c axis (Lc).
In the second part, we utilize potassium hydroxide to chemically activate soft carbons to generate micropores and/or latent pore structures to enhance the electrochemical performances, such as specific capacitance, reversibility, high-rate capability, etc. From the results, the soft carbon after KOH activation, denoted as alkali-soft carbon, is very sensitive to the electrochemical activation; i.e., the specific capacitance of alkali-soft carbon can be dramatically enhanced after the first charge procedure. The above results suggest that electrochemical activation is effective to create the active site for ion intercalation/de-intercalation or adsorption/de-sorption in the graphite-like microcrystalline structure. The alkali-soft carbon with electrochemical activation shows the typical capacitive behavior in the highly positive potential region (-0.6 - 1.4V).
Note that the BET surface area of alkali-soft carbon is very small even though the soft carbon had been activated by KOH. This phenomenon disagrees with the traditional charge storage mechanisms of EDLC. There is a considerable advantage of the low surface area of EDLC electrode material that could avoid the side reaction occurring between electrode material and electrolyte. The lower surface area is, the less possibility of water adsorption on the carbon surface is obtained. Therefore, it could save the cost of the drying process that always occupies the massive part of the total outlay. So far when the positive potential window of alkali-SA03 is 2.6 V (-0.6 - 2.0V), the specific capacitance reaches 65 F g-1. Thus, the alkali-soft carbon could be a superior and novel positive electrode material for high-voltage supercapacitors.
In the final part, it is necessary to utilize design of experiments to obtain the best parameters of KOH activation and electrochemical activation since there is a correlation between the effect of KOH activation and soft carbon microcrystalline structure. Through the best activation condition, when the positive working potential is 2.0 V (-0.6V - 1.4V), the specific capacitance reaches 100 F g-1 or 65 F cm-3. For an asymmetric supercapacitor system, using alkali-SA04 as a positive electrode and ACS25 activated carbon as a negative electrode, an asymmetric supercapacitor with a cell voltage of 3.8 V is developed, in which the cell-specific capacitance and coulombic efficiency are 30 F g-1 and 95%, respectively. Furthermore, the energy density reaches 58.16 Wh kg-1 and power density is 1.85 kW kg-1.

中文摘要 -------------I
Abstract-------------III
致謝 -------------VI
目錄 -------------VIII
圖目錄 -------------XI
表目錄 -------------XVI
第一章 緒論及文獻回顧-------------1
1-1 電化學原理-------------1
1-1-1 電化學反應系統-------------1
1-1-2 電化學裝置-------------2
1-2 電化學電容器-------------7
1-2-1 傳統電容器之簡介-------------7
1-2-2 電化學電容器-------------8
1-2-3 電化學電容器的分類-------------11
1-2-3-1 電雙層電容器-------------11
1-2-3-2 贗電容電化學電容器-------------15
1-3 碳電極材料-------------17
1-3-1 活性碳製備-KOH活化-------------19
1-3-2 軟碳-------------24
1-3-3 電化學活化-------------28
1-3-4 奈米門碳（Nanogate carbon®）-------------31
1-3-4-1 奈米門碳的結構與性能-------------31
1-3-4-2 奈米門碳的電化學活化-------------32
1-3-4-3 奈米門碳的儲能原理-------------34
1-3-5 碳材料微觀結構對電容性能的影響-------------38
1-3-5-1 比表面積與孔徑大小-------------38
1-3-5-2 結構因子-------------42
1-4 有機相高電壓超級電容器-------------45
1-4-1 高電壓電解液(high-voltage electrolyte)-------------48
1-4-2 碳材料的表面改質(surface functional group)-------------52
1-4-3 鈍化膜的形成(passivation film)-------------57
1-4-4 混合型電容器(hybrid capacitors)-------------58
1-5 實驗設計法-------------63
1-5-1 前言-------------63
1-5-2 部分因素設計法(Fractional Factorial Design)-------------64
1-5-3 應答曲面設計(response surface method)-------------68
1-6 研究動機-------------70
第二章 實驗方法與步驟-------------72
2-1 實驗藥品與儀器-------------72
2-1-1 實驗藥品-------------72
2-1-2 實驗儀器-------------73
2-2 碳電極的製備-------------74
2-3 電解液製備及電化學裝置設計-------------75
2-4 電化學及儀器分析-------------75
2-4-1 電化學分析-------------75
2-4-2 儀器分析-------------76
2-4-2-1 掃描式電子顯微鏡(Scanning Electron Microscope, SEM)-------------76
2-4-2-2 X光繞射分析(X-ray diffraction analysis, XRD)------------77
2-4-2-3 氮氣吸脫附曲線-------------79
2-4-2-4 拉曼散射光譜（Raman-------------86
2-4-2-5 X射線光電子能譜學(X-ray photoelectron spectroscopy)-------------87
第三章 不同微晶軟碳應用於正極之行為-------------89
3-1 前言-------------89
3-2 實驗方法-------------89
3-3 不同微晶軟碳的材料分析-------------90
3-3-1 X-ray繞射圖-------------90
3-3-2 SEM影像-------------92
3-3-3 氮氣吸脫附法-------------94
3-3-4 Raman光譜-------------97
3-4 不同微晶軟碳的電化學行為-------------100
3-4-1 循環伏安法 -------------100
3-4-2 等電流充放電-------------104
3-5 不同微晶軟碳在高電壓活化後的材料分析-------------107
3-5-1 SEM影像-------------107
3-5-2 X-ray繞射圖-------------108
3-5-3 Raman光譜-------------111
3-6 小結-------------113
第四章 KOH化學活化軟碳應用於正極之行為-------------115
4-1 前言-------------115
4-2 實驗方法-------------116
4-3 KOH活化軟碳的電化學行為-------------117
4-3-1 循環伏安法及等電流充放電-------------117
4-3-2 嵌入起始電位及不同活化上限電位的影響-------------120
4-3-3 不同KOH活化軟碳微晶結構的影響-------------123
4-4 KOH活化軟碳的材料分析-------------125
4-4-1 SEM影像-------------125
4-4-2 氮氣吸脫附法-------------126
4-4-3 Raman光譜-------------128
4-4-4 X-ray繞射圖-------------130
4-4-5 XPS分析-------------133
4-5 電化學活化機制-------------137
4-6 小結-------------141
第五章 以實驗設計法控制KOH活化軟碳之電容表現-------------143
5-1 前言-------------143
5-2 實驗方法-------------143
5-3 24全因素實驗設計法-------------144
5-4 變異數分析(Analysis of Variables, ANOVA)-------------147
5-5 陡升/陡降實驗(Steepest Ascent/descent Experiment)-------------154
5-6 中央合成設計實驗(Central Composite Design, CCD)-------------156
5-7 非對稱超級電容器之組裝-------------161
5-8 小結-------------165
第六章 結論及未來展望-------------166
6-1 結論-------------166
6-2 未來展望-------------168
參考文獻 -------------176

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