臺灣博碩士論文加值系統

超級電容器為近年來興起的儲能元件，具有比化學電池高的功率密度，優於電容器的能量密度、快速充放電以及更長的循環壽命。可用於各種領域，如電子設備、備用能源、混和動力車能源等。除了電雙層電容器具備之高功率密度特色，在擬電容器方面由於電極表面活性材料之法拉第氧化還原反應所提供的高能量密度也帶來研究的熱潮。超級電容之型態有許多，如對稱超級電容、提高能量密度之非對稱超級電容、用於穿戴式產品的柔性電容以及安全性好之全固態超級電容。
在過去的研究中，常見的電極活性材料如具包含了具備大比表面積的活性碳、介孔碳以及近幾年興起的石墨烯、奈米碳管。其中石墨烯具有優異的導電性、導熱性、大比表面積以及優良的機械性能，但由於其易於堆疊、喪失其表面積優勢，因此尋找適當材料摻雜其中，阻隔自堆疊現象成為近年熱門之課題。
另一方面，為了提高能量密度，研究學者們常使用過渡金屬氧化物，其具備了高理論電容、製作方便、多種樣貌、成本低廉等優點，如四氧化三鈷、四氧化三錳。但金屬氧化物之導電性差、循環穩定性低、元件電阻值高之缺點仍是吾人致力改善的重點之一。
吾人在電泳批複製程中同時添加Graphene、CNT以及Co3O4前驅物，利用夾層創造空間效應製作出具多元孔隙結構之電極材料，大大增加了電泳披覆法的應用潛力。並進一步於製程中加入Mn3O4以提高法拉第電容。結果顯示本研究成功獲得同時具備孔洞式之EPD鍍膜、有效提升功率密度；優良的質傳結構使得擬電容之效能得以發揮。

Supercapacitors is energy storage components that have emerged in recent years, it have higher power density than chemical batteries, and energy density are superior to capacitor , it also have fast charge and discharge, and longer cycle life. It can be used in various fields, such as electronic equipment, backup energy, hybrid vehicle energy, etc. In addition to the physical adsorption/desorption of the electrolyte ions of a typical electric double-layer capacitor, the large capacitance provided by the Faraday redox reaction of the metal oxide on the surface of the material in the pseudo-capacitor also Very popular.
There are many differences about the type of the supercapacitor, such as the most primitive symmetric supercapacitors, asymmetric supercapacitors that increase energy density, flexible capacitors designed to develop wearable products, and solid electrolyte supercapacitors with better safety.
In the past studies, common electrode active materials include activated carbon and mesoporous carbon , which having a large specific surface area. On the other hand , graphene and carbon nanotubes research have risen in recent years. Among them, graphene has excellent electrical conductivity, Thermal conductivity, large specific surface area and excellent mechanical properties. However, due to the graphene will restore back to graphite and loses advantage of large specific surface area. Therefore, find the material doping to block graphene self-stacking has become a hot topic in recent years.
On the other hand , in order to improve the energy density, researchers usually use transition metal oxides, due to its high theoretical capacitance, easy to manufacture, a variety of appearances and low cost.Common metal oxides such as Co3O4 and Mn3O4. However, the poor conductivity of metal oxides, low cycle stability, and high resistance of components are still one of the focuses of researchers.
In this study, we added Graphene, CNT and Co3O4 precursors in the electrophoresis batch replication process, and created the electrode material with multi-porosity structure by using the interlayer to create the spatial effect, which greatly increased the application potential of the electrophoretic coating method. Further, MnO2 was added to the process to increase the Faraday capacitance. The results show that the study successfully obtained the EPD coating with hole type and effectively improved the power density; the excellent quality transmission structure enables the performance of the pseudo capacitor to be exerted.

摘要 I
ABSTRACT II
誌謝 IV
目錄 V
圖表目錄 VIII
第一章 前言 1
第二章 文獻回顧 2
2-1 電化學電容器 2
2-1-1 傳統電容器 2
2-1-2 電雙層電容器 2
2-2 超級電容器 3
2-2-1 超級電容簡介 3
2-2-2 超級電容發展史 5
2-2-3 超級電容儲能機制 6
2-2-3-1 電雙層電容 6
2-2-3-2 擬電容 7
2-2-3-3 混和型電容 8
2-3 電極材料與電解液 9
2-3-1 碳基材料 10
2-3-2 金屬氧化物 11
2-3-3 導電性聚合物 12
2-4 石墨烯 13
2-4-1 石墨烯結構介紹 13
2-4-2 石墨烯製備方式 15
2-4-2-1 微機械剝離法/膠帶法( Micromechanical exfoliation) 15
2-4-2-2 碳化矽表面磊晶法(Epitaxial graphene on SiC) 16
2-4-2-3 化學氣相沉積法(Chemical vapor deposition, CVD) 17
2-4-2-4 氧化石墨化學剝離法 (Graphite oxide chemical exfoliation) 18
2-4-2-5 電化學剝離法(Electrochemical exfoliation) 20
2-4-3 石墨烯應用 21
2-5 奈米碳管 24
2-5-1 奈米碳管結構介紹 24
2-5-2 奈米碳管製備方式 26
2-5-2-1 電弧放電法(arc discharge) 26
2-5-2-2 化學氣相沉積法(chemical vapor deposition) 27
2-5-2-3 雷射蒸發法(laser vaporization) 28
2-5-3 奈米碳管應用 29
2-6 鈷錳氧化物 31
2-6-1 鈷氧化物 31
2-6-2 錳氧化物 34
2-6-3 二元金屬氧化物 36
2-7 電泳沉積 38
第三章 研究方法 40
3-1 實驗藥品 40
3-2 材料分析儀器 42
3-2-1 場發射掃描式電子顯微鏡(Field Emisssion Scanning Electron Microscope，FE-SEM) 42
3-2-2 穿透式電子顯微鏡(Transmission electron microscope，TEM) 43
3-2-3 X-射線繞射儀（X-ray diffractometer，XRD） 44
3-2-4 熱重分析儀(Thermogravimetric analysis，TGA) 45
3-2-5 電化學分析工作站 (Electrochemical workstation) 46
3-2-6 X射線光電子能譜(X-ray photoelectron spectroscopy / XPS) 47
3-3 實驗流程 48
3-3-1 奈米碳管官能化處理 49
3-3-2 鈷氧化物/奈米碳管/石墨烯之水熱合成 50
3-3-3 鈷錳氧化物/奈米碳管/石墨烯製備 52
3-3-4 電泳沉積製備三元複合式電極片 53
3-3-5 電極片電化學分析 54
3-3-6 複合物代號 55
第四章 結果與討論 56
4-1 材料結構之鑑定討論 57
4-1-1 Co3O4/G/C之結晶構造 57
4-1-2 Co3O4/G/C之微觀表面形貌 59
4-1-3 Co3O4/G/C之微結構分析 61
4-2 G/C之不同比例對表面型態暨比電容特性之影響 63
4-2-1 由XRD晶格繞射探討G/C比例之效應 63
4-2-2 由SEM影像探討G/C比例對表面形貌之影響 65
4-2-3 由SEM影像探討添加CNT前後之電極橫截面變化 67
4-2-4 複合材料自身對比電容值之貢獻 68
4-2-5 G/C比例對比電容之影響 70
4-3 CO3O4之含量對表面型態暨比電容特性之影響 73
4-3-1 Co3O4對結晶構造之影響 73
4-3-2 Co3O4含量分析 77
4-3-3 Co3O4含量對表面形貌之影響 79
4-3-4 Co3O4含量對比電容之影響 81
4-4 雙金屬氧化物型超級電容對比電容值之影響 83
4-4-1 Mn3O4之結晶構造 83
4-4-2 Mn3O4之微觀表面形貌 85
4-4-3 不同Co3O4 /Mn3O4添加量對表面形貌之影響 86
4-4-4 Co3O4 /Mn3O4比例對比電容之影響 88
4-4-5 Co3O4 /Mn3O4/G/C電極充放電前後結構變化 91
4-5 全元件測試 92
4-5-1 全元件檢測介紹 92
4-5-2 全元件之電化學特性分析 93
第五章 結論與建議 99
第六章 參考文獻 101

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