本研究旨在製備一具有高熱傳導性質、可撓性，且在熱傳導方向上具有高度異向性之薄膜材料，期望能在電子產業中作熱管理相關應用。為此，本研究以真空抽濾法及水熱還原法製備出石墨烯與奈米碳管(carbon nanotubes, CNTs)複合材料，探討CNT添加量對複合膜熱傳導係數的影響，並分別對平面方向(in-plane)以及垂直平面方向(through-plane)的熱傳導性質做進一步的比較；另外，將複合膜熱壓處理過後，探討熱壓對熱傳值的影響，並進一步作變溫的熱傳導係數量測。研究結果顯示，當CNT添加量越少，在in-plane方向的熱傳值越高，在through-plane方向的熱傳值則越低；經由熱壓後，複合膜於結構及熱傳導方向上的異向性均更為明顯，能有效提升in-plane方向的熱傳值，5 wt% CNT複合膜由787.25 W/m∙K提升至836.80 W/m∙K；而在變溫量測範圍內，in-plane和through-plane的熱傳值均隨著溫度上升而增加，本實驗以5 wt% CNT所製備的複合膜其in-plane熱傳導係數在85 oC時可高達1224.58 W/m∙K為最好的結果，而through-plane方向在 25 oC時為0.058 W/m∙K，在85 oC時達0.080 W/m∙K，代表此材料於不同溫度區間仍具有高度異向性，並達到散熱材料所需高熱傳導性質、可撓性且輕量的薄膜材料之目標。

In order to satisfy the requirement of thermal management of modern electronics, this study aimed to fabricate thin films materials with high thermal conductivity, flexible, and strongly anisotropic heat conduction properties. In this work, we successfully prepared the reduced graphene oxide/multi-walled carbon nanotubes (rGO/CNT) hybrid films with different loadings of CNTs by vacuum filtration and hydrothermal reduction processes, and measured their thermal conductivity by the laser flash method.
The results showed that the film with lower CNT loading possessed higher in-plane but lower through-plane thermal conductivity. After hot-pressed, the anisotropy of both structural and heat conduction properties became more obvious, which can effectively improve the in-plane thermal conductivity from 787.25 W/m∙K to 836.80 W/m∙K for the specimen with 5 wt% CNT loading. As temperature increased, the in-plane thermal conductivity was increased to 1224.58 W/m∙K at 85oC, and the through-plane thermal conductivity was increased from 0.058 W/m∙K at 25oC to 0.080 W/m∙K at 85oC for the specimen with 5 wt% CNT loading, which implies the composites remain highly anisotropic thermal properties at different temperatures studied in this work. The rGO/CNT composites exhibiting high thermal conductivity, flexible, and highly anisotropic thermal properties are promising for heat management applications.

摘要 I
Abstract II
致謝 IV
目錄 VI
表目錄 XI
圖目錄 XII
第一章 緒論 1
1.1 前言 1
1.2 研究動機 2
第二章 文獻回顧 3
2.1 石墨烯的簡介 3
2.1.1 石墨烯的結構 3
2.1.2 石墨烯的特性 4
2.1.3 石墨烯的製備方法 5
2.2 奈米碳管的簡介 9
2.2.1 奈米碳管的起源 9
2.2.2 奈米碳管的結構與性質 10
2.2.3 奈米碳管的製備方法 12
2.3 熱傳導性質的簡介 14
2.3.1 熱傳遞原理 14
2.3.2 熱傳導的量測方法 17
2.3.3 奈米碳材料的熱傳導性質 21
第三章 實驗方法與分析 39
3.1 實驗設備與材料分析儀器 40
3.1.1 電磁加熱攪拌機 40
3.1.2 高速離心機 40
3.1.3 超音波震盪機 41
3.1.4 水循環過濾系統 42
3.1.5 水熱反應爐 42
3.1.6 熱壓機 43
3.1.7 場發射掃描式電子顯微鏡 43
3.1.8 原子力顯微鏡 44
3.1.9 X光繞射分析儀 44
3.1.10 拉曼光譜儀 45
3.1.11 霍式轉換紅外光譜儀 45
3.1.12 雷射閃光法熱擴散係數分析儀 46
3.1.13 四點探針量測儀 47
3.2 實驗步驟及方法 48
3.2.1 製備氧化石墨烯 48
3.2.2 製備氧化石墨烯/奈米碳管混合溶液 49
3.2.3 製備石墨烯及石墨烯/奈米碳管複合膜之試片 50
3.2.4 熱壓石墨烯/奈米碳管複合膜之試片 51
3.3性質分析 52
3.3.1 熱傳導係數量測 52
3.3.2 片電阻量測 53
第四章 結果與討論 64
4.1 石墨烯之分析 64
4.1.1 掃描式電子顯微鏡之形貌觀察 65
4.1.2 原子力顯微鏡形貌分析 65
4.1.3 X光繞射光譜分析 66
4.1.4 拉曼光譜分析 67
4.1.5 霍式轉換紅外光譜分析 68
4.2 奈米碳管之分析 69
4.2.1 掃描式電子顯微鏡之形貌觀察 69
4.2.2 X光繞射光譜分析 70
4.2.3 拉曼光譜分析 70
4.2.4 高解析電子能譜分析(XPS) 71
4.3 石墨烯/奈米碳管複合膜之分析 71
4.3.1 掃描式電子顯微鏡之形貌觀察 71
4.3.2 X光繞射光譜分析 73
4.3.3 拉曼光譜分析 73
4.3.4 霍式轉換紅外光譜分析 74
4.4 熱傳導性質之分析 74
4.4.1 奈米碳管紙之熱傳導係數 75
4.4.2 奈米碳管添加量對熱傳導係數之影響 75
4.4.3 熱壓對熱傳導係數之影響 77
4.4.4 溫度對熱傳導係數之影響 79
4.4.5 熱傳導係數之異向性 80
4.4.6 片電阻之量測 81
第五章 結論 103
參考文獻 105

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