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研究生:王冠穎
研究生(外文):Wang, Guan-Ying
論文名稱:還原氧化石墨烯之薄膜的製備
論文名稱(外文):Preparation of Thin Film with Reduced Graphene Oxide
指導教授:袁維勵
指導教授(外文):Yuan, Wei-Li
口試委員:曾怡享翁于晴
口試委員(外文):Tzeng, Yi-HsiangWeng, Yu-Ching
口試日期:2019-07-16
學位類別:碩士
校院名稱:逢甲大學
系所名稱:化學工程學系
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2019
畢業學年度:107
語文別:中文
論文頁數:85
中文關鍵詞:氧化石墨烯醯胺化界面活性劑
外文關鍵詞:Graphene OxideAmidationSurfactant
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為了改進製作多層結構LED元件所可能遇到的界面問題,本研究提出一種將氧化石墨烯(graphene oxide;GO)經過改質、吸附與化學還原,製備出石墨烯導電薄膜之方法。改質完GO在沉積為薄膜時,可以增進相鄰兩層材料間之附著力。
本研究首先利用大量之油水界面進行接枝反應,同時利用GO表面之-COOH基(羧基)與十二胺(dodecylamine)上之-NH2基(胺基)進行醯胺化反應,將長鏈烷基接枝到GO的其中一個表面,形成片狀GO界面活性劑(GO-surfactant;GO-SFT)。其次利用長碳鏈矽烷偶合劑水解後其上之-OH基(羥基)與自身及ITO玻璃上之-OH基縮合形成化學鍵,使得長碳鏈朝外面形成疏水表面。第三,將GO-SFT分散在水中並將表面疏水化之玻璃基板置入,GO-SFT疏水端將與基板上之疏水端融合,使得GO-SFT之親水面朝外。最後,將吸附有GO-SFT之基板浸泡到聯胺水溶液中,去除GO-SFT之親水官能基,形成還原態之GO(reduced GO;RGO),進而增加石墨烯吸附層之導電性。
先前之研究發現,GO-SFT在水溶液中具有臨界微胞濃度(Critical micelle concentration;CMC),表示可以在水中形成微胞並改變表面張力。本研究成功將GO-SFT吸附到疏水表面上,並還原成RGO,結果製備出大面積石墨烯導電膜。

In order to improve the interface situation that might be encountered in producing multi-layer structured device, a method using graphene oxide (GO) undergoes modification, adsorption and chemical reduction of was proposed in this study to prepare electrically conducting graphene thin films. Modified GO is able to enhance the adhesion between adjacent two layers of different materials when it is deposited as an interfacial layer.
First we used a large amount of oil-water interface to graft long-chain alkyl groups to one side of GO by amidaion reaction of the -COOH groups (carboxyl group) on GO and the -NH2 groups (amine group) of dodecylamine, resulting in planar GO surfactant (GO-SFT). Second, the -OH groups (hydroxyl groups) out of hydrolysis of the silane coupling agent condensed with other wardly, -OH groups of its kind and with those on the ITO glass. The long-chain alkyl groups of silane making the face out making the surface hydrophobic. Third, the GO-SFT is dissolved in water with the hydrophobic substrate immersed. The hydrophobic ends of the GO-SFT were fused with those on the surface so that the hydrophilic ends of GO-SFT face outwardly. Finally, using aqueous hydrazine solution, the hydrophilic functional groups of GO-SFT were removed, rendering reduced GO (RGO), which enhanced the electrical conductance of the adsorbed layer of graphene conductivity is increased.
It was found in previous study that GO-SFT possesses a critical micelle concentration (CMC) in aqueous solution, indicating that it can form micelles in water and change the surface tension. In this study, we successfully adsorbed GO-SFT onto a hydrophobic surface, reduced to RGO, and created a large-area conductive thin film of graphene.

摘要 II
Abstract III
目錄 IV
圖目錄 IX
表目錄 XIII
第一章 緒論 1
1.1 前言 1
1.2 研究動機 2
1.3 石墨烯材料簡介與特性 3
1.3.1 石墨烯的簡介 3
1.3.2 電學特性 4
1.3.3 力學特性 4
1.3.4 熱學特性 5
1.3.5 化學特性 5
1.4 石墨烯的製備方法 6
1.4.1 機械剝離法 6
1.4.2 氧化還原石墨烯法 6
1.4.3 液相剝離法 7
1.4.4 化學氣相沉積法 7
1.5 石墨烯的應用 8
1.6 氧化石墨烯介紹 9
1.6.1 氧化石墨烯發展 9
1.6.2 氧化石墨烯結構 9
1.6.3 氧化石墨烯特性 11
1.6.4 氧化石墨烯應用 12
第二章 文獻回顧 13
2.1 界面活性劑 13
2.1.1 界面活性劑結構與基本性質 13
2.1.2 表面張力 15
2.1.3 臨界微胞濃度(Critical micelle concentration;CMC) 16
2.1.4 界面活性劑的種類 17
2.2 有機發光二極體(ORGANIC LIGHT-EMITTING DIODE; OLED) 20
2.2.1 OLED的發展 20
2.2.2 OLED發光原理 22
2.2.3 OLED優缺點 23
2.3 高分子發光二極體(POLYMER LIGHT-EMITTING DIODE;PLED) 24
2.3.1 PLED的發展 24
2.3.2 PLED發光原理 25
2.3.3 PLED優缺點 25
2.4 矽烷偶合劑(SILANE COUPLING AGENTS) 26
2.4.1 水解反應(Hydrolysis reaction) 26
2.4.2 縮合反應(Condensation reaction) 27
2.5 氧化石墨烯界面活性劑製備 28
2.6 氧化石墨烯還原反應 30
2.7 導電率(ELECTRICAL CONDUCTIVITY) 31
第三章 實驗 32
3.1 實驗藥品 32
3.2 實驗儀器 33
3.3 實驗方法 34
3.3.1 氧化石墨烯製備片狀界面活性劑(GO-SFT) 34
3.3.2 ITO玻璃(玻璃A)表面改質成親油 36
3.3.3 氧化石墨烯吸附在玻璃B上(玻璃C) 39
3.3.4 氧化石墨烯薄膜(玻璃C)還原 41
3.4 實驗分析 43
3.4.1 臨界微胞濃度測量方法 43
3.4.2 傅立葉轉換紅外光譜儀(Fourier-Transform Infrared Spectrometer;FTIR) 44
3.4.3 接觸角測定儀 45
第四章 結果與討論 46
4.1 GO製備片狀界面活性劑(GO-SFT) 46
4.1.1 臨界微胞濃度 46
4.1.2 傅立葉轉換紅外光譜儀 (FTIR) 47
4.2 玻璃A表面改質成親油 49
4.2.1 確認偶合劑是否水解 49
4.2.2 接觸角測定 50
4.3 氧化石墨烯吸附於玻璃B上 51
4.3.1 實驗設計 51
4.3.2 接觸角測定 51
4.3.3 不同浸泡時間下吸附氧化石墨烯界面活性劑程度 52
4.3.4 不同浸泡時間下接觸角測定 53
4.4 氧化石墨烯薄膜還原 54
4.4.1 氧化石墨烯粉末還原 54
4.4.2 氧化石墨烯粉末還原之分散性測試 55
4.4.3 傅立葉轉換紅外光譜儀 (FTIR) 58
4.4.4 RGO導電度測量 60
4.4.5 聯胺對玻璃B接觸角影響 63
第五章 結論 64
參考文獻 65

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