近年來，為因應高功率高能量之儲能需求，新型混合型鋰離子電容器受到學者們關注，其分別由超電容器之正極與鋰離子電池之負極所組成。而鋰離子電容器之負極中最常見之材料為碳材，然而於首次充電時，電解液會於電極材料表面發生化學反應，在負極表面生成鈍化膜，使得溶液中有效鋰離子損失，造成鋰離子電容器效能降低。而預鋰化技術能使負極先生成鈍化膜，並儲存鋰離子，在組裝成鋰離子電容器時，不會使系統內有效鋰離子損失，因此預鋰化技術十分重要。本研究以KOH鹼活化軟碳作為鋰離子電容器之負極碳材，並以電化學預鋰化進行預鋰化，並探討其預鋰化參數。
在預鋰化技術中，電化學預鋰化能精準控制預鋰化程度，但耗時長，因此希望能減少其預鋰化所需之時間。本研究發現，定電壓方法可使預鋰化能更完全，電容量更快達到穩定，使所需循環圈數減少。一般常使用0.1 C進行預鋰化，是因為石墨在低電位時，離子需慢慢擴散至碳層中，而軟碳石墨化程度不完全，具有一定程度之缺陷，故藉由高充放電率使得預鋰化時間減少。但是軟碳於低電位時，鋰離子仍需擴散至碳層內，故在低電位以0.1 C充電，使鋰離子能擴散至碳層中。以預鋰化時間考量，以1 C 充電至0.1 V，再以0.1 C 充電至0.01 V，並於0.01 V定電壓2小時，此兩階段充放電率法，相比傳統預鋰化方法，能減少50 %的預鋰化時間。
由於鹼活化軟碳AlSA04其電容量較低，為了提升鋰離子電容器之電化學表現，希望能使用電容量較高之電極材料，而鹼活化處理使得電容量下降，因此研究未鹼活化處理之軟碳，本研究以四種不同結晶度之軟碳觀察其電容量之影響，從XRD繞射圖與Raman光譜中可以得知四種軟碳具有不同結晶度。而以0.2 C充電、不同充放電率放電下，隨著結晶度愈低，其電容量則愈高；而以相同充放電率充放電之下，在低充放電率下，隨著結晶度愈低，其電容量則愈高；但在高充放電率時，軟碳HCS電容量則最高，其原因為軟碳HCS結晶性較低，鋰離子有足夠之活性位嵌入嵌出，且其層間距也較大，使鋰離子更容易進出碳層，因此在高功率下能有較好的電化學表現。因此軟碳HCS為較適合之負極材料，於10 C時電容維持率相對於0.1 C仍有33 %。
在之前的研究發現鹼活化軟碳AlSA04經由電化學活化後，能有效提升其電容值，經過5.4 V電化學活化後，其於2.0 – 4.6 V時有較高的電容值及庫倫效率，最後將軟碳HCS作為負極與鹼活化軟碳AlSA04作為正極組成鋰離子電容器，並以高充放電率下之電容量進行電量平衡，在正負活性材料重量比0.9時，與MCMB / AlSA04鋰離子電容器比較，可以發現在低功率下，兩者皆無太大差異，但當功率提升至10 kW kg-1時，MCMB / AlSA04 幾乎無法儲能，而HCS / AlSA04則仍有能量密度10 Wh kg-1。
最後將預鋰化電位控制於0.01 V，使鋰離子充份儲存於負極材料中，在功率密度10 kW kg-1時，其能量密度高達30 Wh kg-1，且在500 mA g-1下，相對於第一圈，仍具有90.2%的能量密度維持率，有一定程度的循環壽命，凸顯HCS / AlSA04鋰離子電容器在高功率下之優勢。

In this study, KOH-alkali soft carbon was used as lithium-ion negative carbonaceous material. Soft carbons are low-specific surface area materials, and its effective surface increases via alkali activation. With various prelithiation parameters for prelithiation of the negative electrode, electrochemical prelithiation has been discussed.
For prelithiation, the constant voltage method can improve the charging process and prelithiation, making the capacity more stable, and also reducing the required number of cycles. Since the degree of graphitization of soft carbon is incomplete, the prelithiation time is reduced by charging at high C-rate. However, at lower potential, lithium-ions still need to diffuse slowly into the carbon layers, so the charging rate at lower potential should decrease to 0.1 C. Considering the prelithiation time, the soft carbon is charged to 0.1 V at 1 C and charged to 0.01 V at 0.1 C with constant voltage at 0.01 V for 2 hours. This method, two-step C-rate method can reduce 50% prelithiation time at the 1st cycle compared to traditional method.
Due to the low capacity of alkali-soft carbon AlSA04, the soft carbons with different crystallinity were studied in order to improve the capacity of the negative electrode. From the XRD diffraction pattern and Raman spectra, we can know that these four soft carbons have different microcrystal structure. The discharging ability was studied for four soft carbons with different crystallinity at various discharging rates. At low C-rate, as the crystallinity is lower, the capacity is higher. However, at high C-rates, the capacity of soft carbon HCS is the largest, because of the low crystallinity, which has enough active sites for lithium-ions to intercalate/de-intercalate, and broader interlayer spacing that makes lithium-ions easier to intercalate/de-intercalate into the carbon layers. Even at 10 C, it also has 33% capacity retention rate corresponding to 0.1 C. To assembly lithium-ion capacitors, which need to be charged and discharged quickly, soft carbon HCS is more suitable material.
Compared with MCMB anode, the utilization of HCS anode can obviously improve the specific power of LIC device. When the AlSA04 as cathode is coupled with HCS with prelithiation potential of 0.01 V as anode, the LIC device shows the optimal electrochemical performance, high specific energy up to 30 Wh kg-1 and specific power as high as 10 kW kg-1 (based on active material mass of two electrodes), excellent specific energy retention of 90.2 % after 5,000 cycles. This work indicates the advantages of HCS / AlSA04 lithium-ion capacitors of high specific power and long cycle time.

摘要 I
Abstract III
致謝 V
目錄 VI
圖目錄 i
表目錄 viii
第一章 緒論 1
1-1 電化學電容器 1
1-1-1 傳統電容器 1
1-1-2 電化學電容器 3
1-1-2-1 電雙層電容器 4
1-1-2-2 擬電容電化學電容器 6
1-1-2-3 混合型電化學電容器 8
1-1-3 鋰離子電容器 9
1-2 鋰離子電容器之負極碳材 13
1-2-1 石墨 15
1-2-2 非晶型碳材 18
1-2-2-1 硬碳 19
1-2-2-2 軟碳 21
1-2-3 碳材鹼活化處理 25
1-3 預鋰化 28
1-3-1 化學預鋰化 31
1-3-2 電極添加物預鋰化 32
1-3-3 直接接觸預鋰化 33
1-3-4 電化學預鋰化 34
1-4 研究動機 37
第二章 實驗方法與步驟 44
2-1 實驗方法與儀器 44
2-1-1 實驗藥品及材料 44
2-1-2 實驗儀器 46
2-2 儀器和電化學分析 48
2-2-1 儀器分析 48
2-2-1-1 場發射式掃描電子顯微鏡 48
2-2-1-2 X-ray繞射分析儀 50
2-2-1-3 氮氣吸脫附曲線 52
2-2-1-4 拉曼光譜 55
2-2-1-5 X射線光電子能譜 56
2-2-2 電化學分析方法 58
2-3 鹼活化軟碳之製備 60
2-4 電極製備 61
2-4-1 負極製備 61
2-4-2 正極製備 61
2-5 電化學系統之組裝 62
第三章 軟碳於負極之電化學表現 63
3-1 鹼活化軟碳之材料分析 63
3-1-1 X-ray繞射圖譜分析 63
3-1-2 Raman光譜 66
3-1-3 SEM 影像分析 68
3-1-4 氮氣吸脫附曲線分析 70
3-1-5 XPS光譜分析 72
3-2 循環伏安法 74
3-3 黏著劑之影響 76
3-4 負極預鋰化 79
3-4-1 預鋰化方法 79
3-4-2 定電壓方法 82
3-4-3 不同充放電率 84
3-4-4 不同電位 86
3-4-5 高充放電率充電與定電壓方法 88
3-4-5-1 不同定電壓時間 88
3-4-5-2 不同充放電率 91
3-4-6 充放電率測試 95
3-5 小結 96
第四章 不同微晶軟碳於負極之行為 97
4-1 不同微晶軟碳之材料分析 97
4-1-1 X-ray繞射圖分析 97
4-1-2 Raman 光譜分析 101
4-1-3 SEM 影像分析 103
4-1-4 氮氣吸脫附曲線分析 105
4-1-5 XPS光譜分析 108
4-2 不同微晶軟碳之電化學行為 111
4-2-1 循環伏安法 111
4-2-2 循環壽命圖 115
4-2-3 充放電率圖 117
4-2-4 鋰離子電容器 120
4-2-4-1 鹼活化軟碳於正極之電化學活化表現 120
4-2-4-2 正負極活性材料重量比 124
4-2-4-3 預鋰化電位 144
4-3 小結 147
第五章 結論與未來展望 150
5-1 結論 150
5-2 未來展望 153
參考文獻 154

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