博碩士論文 101329004 詳細資訊




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姓名 黃柏菱(Po-ling Huang)  查詢紙本館藏   畢業系所 材料科學與工程研究所
論文名稱 離子液體電解質應用於石墨烯超級電容之特性分析
(Supercapacitor Properties of Graphene Nanosheets in Ionic Liquid Electrolytes)
相關論文
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★ 以電化學沉積法製備奈米氧化釩及錫在多孔鎳電極上與其儲電特性★ 以超臨界流體製備石墨烯/金屬複合觸媒並 探討其添加對氫化鋁鋰放氫特性的影響
★ 溶劑熱法合成三硫化二銻複合材料應用於鈉離子電池負極★ 利用超臨界流體製備二氧化錫/石墨烯奈米複合材料 應用於鈉離子電池負極
★ 電解質添加劑對鋅二次電池陽極電化學性質的影響★ 電化學法所製備石墨烯及其硼摻雜改質之 超級電容特性分析
★ 氫化二氧化鈦作為鋰、鈉、鎂鋰雙離子電池電極活性材料之電化學性質研究★ 活性碳之粒徑與表面官能基以及所搭配的電解質配方對超高電容特性之影響
★ 超臨界CO2合成SnO2、CoCO3與石墨烯複合材之儲鋰特性及陽極沉積層狀V2O5之儲鈉特性研究★ 高濃度電解質於鋰電池知應用研究
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★ 離子液體電解質於鈉離子電池之應用★ 研發以二氧化錫為負極材料的鈉離子電池: 電解液、輔助性碳材料與黏著劑的優化
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摘要(中) 本研究主要是利用Staudenmaier法製備石墨烯,用來做為超高電容器的電極,電解液則是選用擁有廣大電位窗的離子液體,藉以得到高的能量密度以及功率密度。
首先選用每分鐘1℃升溫到300℃並無持溫的石墨烯 (GNS-300)在不同離子液體內進行比較,使用的離子液體分別為1-ethyl-3-methylimidazolium bis(trifluoromethylsulfony)imide (EMI-NTf2)、N-butyl-N-methylpyrrolidinium bis(trifluoromethylsulfony)imide (BMP-NTf2)、1-ethyl-3-methylimidazolium tetrafluoroborate (EMI-BF4)、1-ethyl-3-methylimidazolium dicyanamide (EMI-DCA) 以及N-butyl-N-methylpyrrolidinium dicyanamide (BMP-DCA),結果顯示在低速充放電下的比電容值與離子液體中的陰離子有關,且在DCA系列的離子液體中具有較佳的比電容值,其中以BMP-DCA的比電容值為最高,約234 F/g左右, 若陰離子相同,在高速充放電下,EMI系列的比電容值皆高於BMP系列的比電容值,但因BMP-DCA的電位窗可達3.3 V,而EMI-DCA只有2.5 V,所以其能量密度 (88.5 Wh/kg)以及功率密度 (17.1 kW/kg)皆高於EMI-DCA,所以便選用BMP-DCA做為電解液。
目前碳材皆以多孔碳材方向發展,但製程皆過於繁複,本研究期望利用簡便的熱還原法,利用不同升溫速率製造孔洞,以及升溫至不同溫度比較含氧官能基對於石墨烯之影響。本研究選用五種碳材在離子液體BMP-DCA中進行比較,石墨烯方面,選用三種情況下製程之石墨烯進行比較,分別是GO放入300 ℃的高溫爐並無持溫 (多孔含氧官能基多石墨烯,HGNS-300)、每分鐘升溫1℃直到300℃並無持溫 (無孔洞含氧官能基多石墨烯,GNS-300)以及每分鐘升溫60℃直到1100℃並無持溫(多孔含氧官能機少石墨烯,HGNS-1100),另外兩種則分別為活性碳 (Activated carbon)以及多壁奈米碳管 (Multiwalled Carbon Nanotubes),根據結果顯示,多孔含氧官能基多石墨烯的比電容值高於其他碳材,並且擁有高的比電容值 (327 F/g)、能量密度 (123.7 Wh/kg)以及高的功率密度 (17.3 kW/kg)。兩千圈後維持率仍有79 %。目前超高電容普遍是以活性碳在有機中為主軸,本研究比較多孔含氧官能基多石墨烯以及活性碳在有機溶液TEABF4/PC以及離子液體BMP-DCA的超高電容行為,由結果得知多孔含氧官能基多石墨烯在離子液體BMP-DCA中有最好的超高電容性能。在高溫60 ℃下比較BMP-DCA以及TEABF4/PC,由結果得知高溫下有機溶液性能提升不多,而離子液體的性能大幅提升,其比能量密度由123.7 Wh/kg提升為138.8 Wh/kg,比功率密度則由17.3 kW/kg提升為51.6 kW/kg。
摘要(英) The graphene sheets were prepared by Staudenmaier method in this study, and were used for the electrode in supercapacitor. We chose ionic liquids as electrolyte for their wide potential window to get better energy density and power density.
First we chose graphene (GNS-300) which is made by raising temperature 1℃ per 1 min to 300°C. We used this GNS-300 to test in different ionic liquids, and compare their properties. The ionic liquids included EMI-NTf2, BMP-NTf2, EMI-BF4, EMI-DCA, and BMP-DCA. The results showed that the specific capacitance at low scan rate was related to the anion of ionic liquids. And the graphene sheets in the DCA-based ionic liquids had the best capacitance performance. In particular, in BMP-DCA, the specific capacitance of graphene sheets was 234 F/g. At high scan rate, EMI-NTf2 and EMI-DCA have higher specific capacitance than BMP-NTf2 and BMP-DCA. But the potential window of graphene sheets in BMP-DCA was 3.3 V, it’s bigger than EMI-DCA, so BMP-DCA can get better enrgy density for 88.5 Wh/kg and power density for 17.1 kW/kg.
In my research, we want to use thermal reduction to change different raising temperature rate and different temperature. We hope that we can get holes and oxygen containing groups to improve graphene’s superapacitor performance. So we choosing five carbon materials to compare in BMP-DCA. We chose three kinds of graphene sheets like HGNS-300 which is made by raising temperature to 300°C directly, GNS-300 which is made by raising temperature to 300°C per 1°C per 1min, and HGNS-1100 which is made by raising temperature to 1100°C per 60°C per 1min. The other carbon materials were activated carbon (AC) and multiwalled carbon nanotubes (MWCNT). The studies showed HGNS-300 had the highest specific capacitance than others because HGNS-300 had holes and many oxygen containing functional group. HGNS-300 had highest specific capacitance of 327 F/g, energy density of 123.7 Wh/kg and power density of 17.3 kW/kg. After 2000 cycles, the retention still have 79 %. Compare HGNS-300 and activated carbon in BMP-DCA and TEABF4/PC, we can get that HGNS-300 in BMP-DCA have best supercapacitor performance. Compare HGNS-300 in BMP-DCA and TEABF4/PC at 60 ℃, the results show that test in BMP-DCA, getting better energy density for 138.8 Wh/kg and power density for 51.6 kW/kg.
關鍵字(中) ★ 超高電容器
★ 石墨烯
★ 離子液體
關鍵字(英)
論文目次 摘要 i
ABSTRACT iii
誌謝 v
目錄 vii
表目錄 xi
圖目錄 xiii
第一章、 前言 1
第二章、文獻回顧 3
2-1能源儲存裝置概述 3
2-2 超高電容器簡介 7
2-2-1電雙層電容器 (electric double-layer capacitors) 8
2-2-2擬電容器 (pseudo-capacitors) 11
2-3電雙層電容器之材料分類 14
2-4石墨烯之材料特性與製備方法 17
2-4-1石墨烯之材料特性 17
2-4-2石墨烯之製備方法 20
2-5超高電容器之電解質 25
2-6以離子液體做為電解質之超高電容器 31
第三章、實驗步驟 43
3-1 碳材之準備 43
3-1-1石墨烯之製備 43
3-1-2多壁奈米碳管之取得 44
3-1-3活性碳之取得 44
3-2電解液之製備 45
3-2-1合成BMPC (1-Butyl-1-methylpyrrolidinium Chloride) 45
3-2-2合成離子液體 46
3-3 材料特性分析 48
3-3-1表面形貌之觀察 48
3-3-2表面組成以及缺陷結構 48
3-3-3結晶結構分析 48
3-4 碳材於離子液體內電化學性質之評估 49
3-4-1電極之製備 49
3-4-2電化學裝置 49
3-4-3電化學性質之評估 50
第四章、結果與討論 53
4-1石墨烯 (GNS-300)於不同離子液體內之比較 53
4-1-1石墨烯之材料特性分析 53
4-1-2 離子液體之電化學性質 54
4-1-3石墨烯 (GNS-300)於EMI-NTf2中之電雙層電容行為 54
4-1-4石墨烯 (GNS-300)於BMP-NTf2中之電雙層電容行為 55
4-1-5石墨烯 (GNS-300)於EMI-BF4中之電雙層電容行為 56
4-1-6石墨烯 (GNS-300)於EMI-DCA中之電雙層電容行為 57
4-1-7石墨烯(GNS-300)於BMP-DCA中之電雙層電容行為 58
4-1-8石墨烯 (GNS-300)於不同電解液之儲電性能 59
4-1-9石墨烯 (GNS-300)與活性碳於有機溶液以及離子液體之比較 64
4-1-10石墨烯(GNS-300)於有機溶液以及離子液體不同溫度之比較 65
4-2不同碳材於離子液體BMP-DCA中之比較 93
4-2-1不同碳材表面形貌之觀察 93
4-2-2不同碳材表面組成以及缺陷結構 94
4-2-3不同碳材結晶結構分析以及比表面積分析 95
4-2-5離子液體BMP-DCA 96
4-2-6不同碳材於離子液體BMP-DCA中之儲電性能 97
4-2-7多孔含氧官能基多石墨烯 (HGNS-300)與活性碳於有機溶液以及離子液體之比較 102
4-2-8多孔含氧官能基多石墨烯 (HGNS-300)於有機溶液以及離子液體不同溫度之比較 104
第五章、結論 127
參考文獻 129
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指導教授 張仍奎(Jeng-kuei Chang) 審核日期 2014-8-21
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