本論文以化學氧化合成法製備不同碳材與聚砒硌複合材料，包括還原氧化石墨烯/碳奈米管/聚砒硌(rGO/CNT/PPy)、碳奈米管/聚砒硌(CNT/PPy)及活性碳/聚砒硌(AC/PPy)複合材料，並系統性了解最佳組成比例以及在水相與有機相電解液的電化學特性。碳材形貌決定聚砒硌複合材料形貌進而影響電化學特性與特徵，rGO/CNT/PPy具有較佳的電容表現，於水相與有機相電解液之負電位下限分別延展至-0.8 V (vs. Ag/AgCl)與-2.5 V (vs. Ag/AgNO3, acetonitrile)。水相含鉀離子電解質可有效提升rGO/CNT/PPy電化學的可逆性與穩定性，水合離子半徑亦影響材料的電容性能表現如比電容值、氧化還原可逆性以及功率性能。另外電極配方導入碳黑(XC-72)有助於提高壽命與循環穩定性以及提升材料電化學性能。於有機相之不同極性電位窗循環測試以及水相的偏壓測試，皆說明rGO/CNT/PPy適合作為非對稱電容器之負極。以Mn3O4作為正極材料和rGO/CNT/PPy作為負極材料所組立之水相非對稱超級電容器，其電池電壓可達1.8 V，比能量與比功率性能為17.3Wh kg-1和7.36 kW kg-1。此非對稱超級電容器在電池電壓1.6 V展現理想的電容行為與卓越充放電循環穩定性，即便經過3250循環充放電次數，仍維持一樣的電容量性能。

Using chemical oxidation method, polypyrrole(PPy) has been polymerized onto different carbon materials including reduced graphene oxide/carbon nanotube (rGO/CNT), carbon nanotube (CNT) and activated carbon (AC), to form three composites that are denoted as rGO/CNT/PPy, CNT/PPy, and AC/PPy. The electrochemical characteristics of the above composites in aqueous electrolytes and organic electrolytes are systematically studied for the supercapacitor application. The morphologies of these composites depend on the shape of carbons and affect their electrochemical performance. The rGO/CNT/PPy provides higher specific capacitance than the others and its negative potential limit can be extended to -0.8 V (vs. Ag/AgCl) and -2.5 V (vs. Ag/AgNO3, acetonitrile) in aqueous electrolyte (0.5 M Na2SO4) and organic electrolyte (1M TEABF4/PC), respectively. The rGO/CNT/PPy shows improved reversibility and higher stability in the aqueous electrolyte containing K+. In addition, the introduction of carbon black (XC-72) into electrode preparation has been found to enhance the specific capacitance and the cycling stability.
The galvanostatic charge/discharge cycle test with different positive and negative potential ranges in the organic electrolyte as well as the potential-bias stress test under different positive and negative potentials in various aqueous electrolytes are employed to confirm the stability of the rGO/CNT/PPy composite. As a result, this composite is a suitable negative electrode material for the asymmetric supercapacitor.
Finally, an asymmetric supercapacitor (ASC) with a positive electrode of Mn3O4 and a negative electrode of rGO/CNT/PPy is successfully demonstrated, which shows specific energy and power of 17.3 Wh kg-1 and 7.36 kW kg-1 with a cell voltage of 1.8 V. This ASC with a cell voltage of 1.6 V shows excellent charge-discharge cycle stability and ideal capacitive behavior in NaNO3 even after the application of 3250 charge-discharge cycles.

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