懸空石墨烯之特性研究與應用

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姓名

陳祐民(Yu-Min Chen) 查詢紙本館藏

畢業系所

機械工程學系

論文名稱

懸空石墨烯之特性研究與應用
(Characterizations of Suspended Graphene Film and its Applications)

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★ 化學氣相沉積法合成二硫化鉬於矽基材料之可控性及變異性研究	★ 使用低損傷電漿改質於提升二維通道電晶體電傳輸特性
★ 利用電化學剝離石墨烯之三維多孔隙電極於製作可撓式超級電容	★ 結合分子臨場吸附與電化學剝離法製備高品質石墨烯

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摘要(中)

石墨烯為單一原子層的二維材料，具有優異的材料性質包含：高光穿透率、可彎折、高熱傳導、電傳導等性質，近年來石墨烯的相關研究發展相當快速，但大多數元件都需基板支撐，當石墨烯薄膜被基板支撐時，基板會參與石墨烯的聲子、電子等粒子的傳遞，導致無法呈現本質石墨烯性質，因此石墨烯懸空便成為實現常溫下超高速元件的一個選擇；但目前單層石墨烯以背向漂浮法能懸空的尺度為直徑500μm，製程複雜不穩定且容易於附著高分子殘留物。本研究主要發展一種簡易且可靠的方法來研製大面積的懸空石墨烯。首先，將銅箔基板藉由電化學拋光後，以常壓化學氣相沉積法進行成長，改變氫氣流量得到高品質單層石墨烯薄膜，其製程優化之單晶高品質石墨烯的晶粒可達~50μm。第二部分將單層石墨烯堆疊五層並以熱裂解法進行轉印，得到最大尺度可達1,500μm石的懸空墨烯薄膜，成功懸空的比率皆較背向漂浮法提高200%，且能排除高分子殘餘物的影響，氧化基團鍵結分別下降4～6%不等，載子遷移率提高154%。此外，本研究也演示了電容式壓力感測器的應用，結果顯示電容值與壓力變化具有良好的線性趨勢，而其感測之靈敏度為15.15aF/Pa，相對於矽基材料提升達七倍(~770%)，基於此種懸空結構的製程，在未來將可望應用於微機電和生醫感測器、高頻電子元件等廣泛的應用。

摘要(英)

Graphene is a one atom thickness 2D material that shows remarkable material properties, including high optical transparency, mechanical flexibility, high thermal conductivity, and superior high conductivity. In the last decade, graphene research and its related applications have been attracted intensive attentions. However, the earlier research on graphene device were performed on substrate. The substrate induced carrier scattering, charge impurity doping and corrugation that drastically degrade the intrinsic properties of graphene. Thus the suspended graphene shows superior intrinsic material properties on carrier transport, thermal conductivity and mechanical elasticity. Especially the practical application in ultra-high speed device. Before this study, the suspended graphene membrane made by the inverted floating method can yield the large size about 500μm in diameter; however, the suspended graphene by this approach were suffered from issues of the difficulty for manipulation and complicated process as well as the large amounts of polymer residue on graphene. This study was to develop a simple and reliable route to achieve a large area of suspended graphene. The proposed process including (1) the optimization of graphene growth conditions by atmospheric pressure chemical vapor deposition (APCVD) and (2) the transferring process for suspended graphene by solvent replacing and thermal decomposition method. It was found out that the optimized graphene single crystalline size with high quality could be up to ~50μm. The results shows that the largest suspended graphene membrane over 1,500μm in diameter can be obtained by stacking and transferring 5-layered graphene on a holy substrate. The XPS characterization shows that the extremely low oxygen functional groups of 4～6% on graphene membrane after thermal annealing can be achieved, suggesting the ultra-clean and high quality of suspended graphene can be made from our approach. To study the intrinsic properties and application of our suspended graphene membrane, the devices integrated with suspended graphene were fabricated. The results shows that the carrier mobility on suspended graphene is enhanced up to 154% when compared with the substrate supported graphene. In addition, the capacitive pressure sensor made by our ultra-large suspended graphene membrane, showing a superior high sensitivity and excellent signal linearity than conventional capacitive pressure sensors. The sensitivity of 15.15 aF / Pa were measured which is increased about 422~ 770% than silicon-based material. The developed method for ultra-large suspended graphene pave the way for the potential applications on electromechanical actuator, ultra-sensitive chemical/bio sensors as well as the high-frequency electronic devices.

關鍵字(中)

★ 石墨烯
★ 懸空石墨烯
★ 化學氣相沉積
★ 轉印
★ 電容式壓力感測器

關鍵字(英)

★ Graphene
★ Suspended Graphene
★ Chemical Vapor Deposition
★ Transfer
★ Capacitive Pressure Sensor

論文目次

頁次
中文摘要 i
英文摘要 ii
誌謝 iv
目錄 v
表目錄 viii
圖目錄 ix
第一章緒論 1
1-1文獻回顧 1
1-1-1石墨烯 1
1-1-2單層石墨烯的晶體結構 1
1-1-3石墨烯的材料性質 3
1-1-4石墨烯的應用領域 4
1-1-5石墨烯的製備方式 4
1-1-6片層微縮機制 5
1-1-7自組裝成長機制 11
1-1-8石墨烯的轉印製程 16
1-1-9捲對捲連續合成石墨烯之製程 20
1-1-10單晶石墨烯 22
1-2懸空石墨烯的物理系性質 24
1-2-1懸空石墨烯的電性 26
1-2-2懸空石墨烯的導熱性 27
1-2-3懸空石墨烯的機械強度 28
1-3懸空石墨烯製備方式 30
1-4懸空石墨烯之應用元件 34
1-4-1過濾膜 34
1-4-2壓力感測器 35
1-5實驗動機 37
第二章實驗設備 38
2-1各類實驗藥品、氣體清冊 38
2-2高溫爐管及真空系統 39
2-3旋轉塗佈機 39
2-4表面分析儀器 40
2-4-1 二維表面粗度量測儀 40
2-4-2掃描式電子顯微鏡 40
2-4-3穿隧式電子顯微鏡 40
2-4-4原子力顯微鏡 40
2-4-5接觸角量測儀 41
2-5光學分析儀器 41
2-5-1紫外光/可見光/近紅外光譜儀 41
2-5-2拉曼光譜儀 41
2-6 電性分析 42
2-6-1霍爾量測儀 42
2-6-2電感、電容、電阻量測儀 42
2-6-3四點探針量測儀 42
2-7元素分析 43
2-7-1 X光電子能譜儀 43
第三章實驗架構與流程 44
3-1製程步驟 45
3-1-1銅基板之電解拋光平坦化 45
3-1-2單晶石墨烯成長 45
3-1-3單晶石墨烯轉印 47
3-1-4石墨烯完整成長 48
3-1-5多層堆疊石墨烯 49
3-1-6製備懸空石墨烯 50
3-1-7懸空石墨烯之壓力感測元件製作 52
3-1-8懸空石墨烯元件之電容值量測 52
第四章結果與討論 53
4-1電解拋光對於銅箔表面粗糙度之優化參數探討 53
4-2單晶石墨烯成長結果 55
4-2-1石墨烯統單晶尺寸統計定義 55
4-2-2單晶石墨烯成長結果之表面形貌分析 56
4-3石墨烯連續薄膜成長 65
4-4多層堆疊石墨烯 69
4-5懸空多層石墨烯 72
4-5-1清洗溶劑接觸角量測 72
4-5-2懸空石墨烯製備方法比較 73
4-5-3完成懸空成功率比較 75
4-5-4多層石墨烯之拉曼光譜圖 76
4-5-5霍爾量測 78
4-5-6 X射線光電子能譜圖 80
4-5-7懸空石墨烯電容值 82
4-6 本實驗與其他工作之結果比較 84
第五章結論 85
第六章未來展望 86
參考文獻 87

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IEEE Industrial Electronics, IECON 2006 - 32nd Annual Conference, p.3166 - 3169

指導教授

蘇清源(Ching-Yuan Su)

審核日期

2015-10-2

推文