超級電容器的電極材料及電解質是決定效能的關鍵。為了提升超級電容器的應用範圍及性能表現，可藉由開發階層狀孔洞碳材、發展離子液體電解質系統、改良碳電極結構等方式，提高電容器的操作電位窗、儲能密度、輸出功率及循環壽命，突破現階段電容元件的能量儲存極限及操作限制。
　　本論文分為三部份：(1) 階層狀(Hierarchical)孔洞活化介相瀝青碳材(Activated mesophase pitch, aMP)搭配離子液體組裝成具高能量密度之電雙層電容器(Electric double layer capacitors, EDLCs); (2) 醚基架橋雙陽離子離子液體(Ether-bridged dicationic ionic liquid)應用於寬工作溫度範圍之電雙層電容器; (3) 階層狀孔洞碳材搭配雷射微刻技術組裝成高能量與功率密度之微型超級電容器(Microsupercapacitors)。
　　第一部份，電雙層電容器使用兩種離子液體:1-ethyl-3-methylimidazolium and 1-methyl-1-propylpyrrolidinium bis(trifluoromethylsulfonyl)imides, EMIm- and MPPy-TFSIs)，可操作的工作電位分別是3.5 V與4.1 V，並分析電荷在電雙層電容器中的儲存行為。高電位操作下，微孔較多的活化介相瀝青碳材和活性碳纖維(Activated carbon fiber, aCF)組裝成對稱型二極式電容器，在循環伏安法分析中都具有典型的電雙層電容行為，不過對於中孔洞碳材(Templated mesoporous carbon, tMC)卻出現電荷遷入的反應波峰。施加高偏壓於交流阻抗分析中，發現中孔碳材的結構較有利於離子傳遞，不過電荷儲存阻力卻較活化介相瀝青和活性碳纖維高。實驗結果指出具有較多微孔的碳材在高電位下，微孔能夠容納單一離子，缺乏微孔的中孔碳材因離子遷入石墨層進而破壞結構。活化介相瀝青碳材具有由中孔與微孔連接而成的階層狀孔洞結構，有利於高電位下做快速充放電。亦具有緊密的石墨層結構，搭配離子液體可提供高能量密度之超級電容器。
　　第二部份，此部分成功合成具有醚基架橋主鏈之雙陽離子離子液體([C6O2(MIm)2]-TFSI2)，當作添加劑添加於EMIm-TFSI中並應用於電雙層電容器，能夠在溫度範圍20 C到60 C間作快速充放電。醚基架橋結構使雙陽離子在形態上更具多異性，因此不具有明顯的凝固點與玻璃轉化溫度。添加於EMIm-TFSI中可使其凝固點下降，並有效降低離子間作用力與提升導離子度。搭配活化介相瀝青碳材組裝成電雙層電容器，可藉由降低電解質離子在電極間的傳導阻力與離子在孔洞內的擴散阻力增加離子的移動速度。放電速率0.5 A g-1，在60 C和20 C下，其電容值能高達208和160 F g-1。在高電位窗3.5 V下，功率20 000 W kg-1時，比能量能高達70 Wh kg-1。[C6O2(MIm)2]-TFSI2與EMIm-TFSI的協同作用(Synergistic effect)完全展現在優異的電化學電容表現上。
　　第三部份，微型超級電容器可作為微型裝置的電力來源與儲能元件。本部分研究先將活化介相瀝青碳材沉積在基材上，再利用雷射微雕刻系統刻劃出指插狀微電極，最後塗佈膠狀電解質(Gel-state electrolytes)形成固態微型超級電容器。因為活化介相瀝青碳材的階層狀結構，有利於高速下做充放電。透過縮小微電極線寬的設計，更進一步降低離子在電極與電極間的傳導阻力與在碳膜內部的擴散阻力。搭配膠態離子液體(Ionogel)電解質，整體元件體積電容高達12 F cm-3，能量密度16 mW h cm-3與功率密度160 W cm-3，這些數值已接近薄膜鋰離子電池與鋁電解電容。此外，此微型超電容也擁有優異的循環充放電次數和熱穩定性。因此，此微型電容器製程的發展不僅簡易與成本低，而且提供更多不同微型儲能裝置的發展空間。

This dissertation includes three parts: (1) Electric double layer capacitors (EDLCs) of high volumetric energy based on ionic liquids (ILs) and hierarchical pore carbon. (2) Ether-bridged dicationic ionic liquid (DIL) applied in a wide temperature range for EDLCs. (3) Laser fabrication of all-solid-state microsupercapacitors (MSCs) with ultrahigh energy and power based on hierarchical pore carbon.
In the first part, we analyze the high-voltage charge-storage behavior of EDLCs in which two IL electrolytes are used, 1-ethyl-3-methylimidazolium and 1-methyl-1-propylpyrrolidinium bis(trifluoromethylsulfonyl)imides (EMIm- and MPPy-TFSIs), and are operated at 3.5 and 4.1 V, respectively. Symmetric two-electrode capacitor cells assembled using micropore-rich activated mesophase pitch (aMP) and activated carbon fiber (aCF) carbons show a standard capacitive behavior in cyclic voltammetry (CV) analysis, whereas cells featuring templated mesoporous carbon (tMC) show ion-intercalating peaks in high-voltage scans. Impedance analysis performed at high voltages reveals that the aMP and aCF cells show lower charge-storage resistance than the tMC, although tMC facilitates ion transport more efficiently than aMP and aCF. The experimental results indicate that micropore-rich aMP and aCF accommodate single ions at high voltages, whereas the carbon structure is destroyed in micropore-deficient tMC because of graphitic-layer intercalation. The aMP carbon, which contains hierarchically connected micropores and mesopores, is effective in storing charge at a high rate at high voltages. Because of the compact feature of aMP, incorporating ionic liquids with aMP represents a very promising strategy for assembling capacitors of ultrahigh volumetric energy densities.
The second part presents the synthesis of a dicationic ionic liquid (DIL) comprising two ethylimidazolium cations linked by an ether-bridged linker and paired with two bis(trifluoromethanesulfonyl)imide anions (i.e., [C6O2(MIm)2]-TFSI2) introduced into 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMIm-TFSI) as an electrolyte for electric double-layer capacitors (EDLCs) operated in a wide temperature range (from -20 to 60 °C). [C6O2(MIm)2]-TFSI2 has a flexible ether-bridged moiety that provides the DIL with a high conformational degree of freedom and suppresses the crystallinity of EMIm-TFSI. The existence of [C6O2(MIm)2]-TFSI2 effectively reduces interionic interaction, thus increasing ionic conductivity. During the assembly of the electrolyte mixture in a porous carbon-based symmetric EDLC, [C6O2(MIm)2]-TFSI2 facilitates ion motion by reducing the ion transport resistance in the bulk electrolyte and the ion diffusion resistance in the pores. At temperatures of 60 and -20 °C, this symmetric EM-di5-EDLC (5 wt% of [C6O2(MIm)2]-TFSI2 in mixture) has high capacitance values of 208 and 160 F g-1, respectively, at a discharge current of 0.5 A g-1. The EM-di5-EDLC can deliver a specific energy of 70 Wh kg-1 at a high power of 20000 W kg-1 over a wide voltage window of 3.5 V. The excellent electrochemical response of the cells indicates the synergistic performance of [C6O2(MIm)2]-TFSI2 and EMIm-TFSI for improving the capacitive energy storage.
In the third part, MSCs are used as power sources or energy storage units in microelectronic devices. This study fabricates all-solid-state MSCs using a laser for the micromachining of substrates coated with aMP to produce in-plane interdigitated microelectrodes for use in conjunction with gel-state electrolytes. Due to the inclusion of hierarchically-connected micropores and mesopores, aMP carbon has considerable capability for charge storage and the delivery of energy at high rates. Through reduction in the finger width, the proposed laser-patterned design substantially reduces the resistance to ion drift in the electrolyte bulk and ion diffusion across the carbon-film network. The use of an ionogel (IG) enables the MSC to reach stack capacitance of 12 F cm-3, stack energy of 16 mWh cm-3, and stack power of 160 W cm-3. These energy and power values approach those obtained from thin-film lithium ion batteries and aluminum electrolytic capacitors, respectively; this synergy between high energy and power is unprecedented for MSCs. The proposed MSCs exhibit outstanding cycling stability and those using IG present high thermal stability. The proposed fabrication methods enable the on-chip integration of microelectronic devices and therefore provide an opportunity for the development of a variety of micro/nano-sized energy devices.

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