臺灣博碩士論文加值系統

本論文係有關使用奈米碳管(CNT)、還原氧化石墨烯(rGO)及其與導電高分子聚二氧乙基噻吩:聚苯乙烯磺酸(PEDOT:PSS)之複合物發展可撓式透明導電電極與超級電容器之研究。首先，利用刮刀塗佈法將CNT及氧化石墨烯(GO)分散液分別塗佈在聚對苯二甲酸乙二酯(PET)上作為可撓式透明導電電極，其中GO薄膜需進一步使用氫碘酸還原，結果顯示穿透度及電阻隨著塗佈層數增加而降低。接著，分別將CNT及GO分散液加入等體積之PEDOT:PSS及DMSO得到含0~0.1wt% CNT或GO的均勻分散液，後者並進一步以微波還原法製得rGO分散液，然後利用刮刀塗佈法將CNT與rGO的分散液分別塗佈在PET表面，製得CNT/PEDOT:PSS 與rGO/PEDOT:PSS複合薄膜作為可撓式透明導電電極，結果發現適量碳材的添加確實能夠建構導電網絡提升導電性，且兩者最低電阻都在1000 Ω左右且穿透度超過80%。最後，研究證實CNT/PEDOT:PSS 和rGO/PEDOT:PSS複合薄膜兩者亦皆可作為超級電容器之電極，且其電容值可隨薄膜厚度之適當增加而提升。此外，進一步使用聚乙烯醇/硫酸(PVA/H2SO4)製得的膠態電解質，分別和兩片CNT/PEDOT:PSS或 rGO/PEDOT:PSS電極組裝成可撓式全固態透明超級電容器，其穿透度皆超過56 %，並具有快速充放電的能力，且其電化學性能在彎折時皆可保留。所有的結果證實CNT/PEDOT:PSS或rGO/PEDOT:PSS可發展作為可撓式全固態透明超級電容器之電極材料。

This thesis concerns the developments of flexible transparent conductive electrodes and supercapacitors using carbon nanotube (CNT), reduced graphene oxide, and their hybrids with conducting polymer poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS). At first, the CNT and rGO-based thin films were fabricated as flexible transparent conductive electrodes by the blade-coating of CNT or graphene oxide (GO) dispersion on polyethylene terephthalate (PET) and the followed GO reduction with hydroiodic acid for the case of GO. The decreases of transmittance and sheet resistance with the increase of layer numbers have been described. Secondly, CNT or GO (0~0.1wt%) was added to the equal volume mixture of PEDOT:PSS and dimethyl sulfoxide (DMSO) to yield homogeneous dispersions. For the case of GO, the dispersion was further microwave-treated to obtain the rGO dispersion. Then, the CNT or rGO dispersion was blade-coated on PET to form the CNT/PEDOT:PSS or rGO/PEDOT:PSS hybrid thin films as flexible transparent conductive electrodes. It was found that the appropriate addition of CNT or rGO indeed could effectively enhance the conductivity via the formation of conductive network. The lowest sheet resistance around 1000 Ω with a transmittance above 80% was obtained for both the hybrid thin films. Finally, it was demonstrated that both the CNT/PEDOT:PSS and rGO/PEDOT:PSS hybrid thin films also could be used as the electrodes for supercapacitors. The capacitance could be raised by appropriately increasing the thickness of hybrid thin films. Furthermore, the flexible transparent all-solid-state supercapacitors were fabricated with polyvinyl alcohol/sulfuric acid (PVA/H2SO4) gel electrolyte between two CNT/PEDOT:PSS or rGO/PEDOT:PSS hybrid thin film-based electrodes. It was found that both the resulting supercapacitors had transmittances above 56% and could be quickly charged and discharged. Also, their electrochemical performance could be retained while bending. All the results revealed that both the CNT/PEDOT:PSS and rGO/PEDOT:PSS hybrid thin films could be developed as good electrode materials for flexible transparent supercapacitors.

中文摘要 I
Abstract II
Extended abstract IV
誌謝 VIII
總目錄 X
圖目錄 XIII
表目錄 XVII

第一章 緒論 1
1.1 石墨烯 1
1.1.1 石墨烯簡介 1
1.1.2 石墨烯製備 3
1.1.3 氧化石墨烯和還原氧化石墨烯 5
1.2 奈米碳管 9
1.2.1 奈米碳管簡介 9
1.2.2 奈米碳管製備 11
1.3 導電高分子 13
1.3.1 導電高分子 13
1.3.2 PEDOT:PSS 15
1.4 超級電容器之簡介 20
1.4.1 超級電容器基本原理 20
1.4.2 可撓式與透明超級電容器 25
1.5 研究動機 29
第二章 基本理論 31
2.1 循環伏安法理論 31
2.2 定電流充放電原理 33
2.3 電化學交流阻抗原理 35
第三章 實驗方法 38
3.1 實驗藥品與儀器 38
3.1.1 藥品 38
3.1.2 儀器 40
3.2 實驗步驟 42
3.2.1 GO製備 42
3.2.2 CNT薄膜製備 43
3.2.3 GO 薄膜製備 44
3.2.4 聯胺還原GO薄膜 44
3.2.5 氫碘酸還原GO薄膜 45
3.2.6 CNT/PEDOT:PSS薄膜製備 45
3.2.7 rGO/PEDOT:PSS薄膜製備 46
3.2.8 電化學測試 47
3.2.9 固態電解質 48
3.2.10 全固態電容器組裝 48
3.2.11 特性分析 49
第四章 結果與討論 51
4.1 可撓式透明導電膜 51
4.1.1 CNT透明導電膜 51
4.1.2 GO及rGO透明導電膜 55
4.1.3 CNT/PEDOT:PSS之可撓式透明導電膜 60
4.1.4 rGO/PEDOT:PSS可撓式透明導電膜 64
4.2 可撓式透明超級電容器 70
4.2.1 CNT/PEDOT:PSS 70
4.2.2 rGO/PEDOT:PSS 75
4.3 可撓式全固態透明超級電容器 80
4.3.1 CNT/PEDOT:PSS 80
4.3.2 rGO/PEDOT:PSS 86
第五章 結論 92
參考文獻 93

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