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研究生:蔡運邦
研究生(外文):Tsai, Yun-Pang
論文名稱:多壁奈米碳管-纖維強化乙烯基樹脂複合材料之製備及其機械性質之研究
論文名稱(外文):Preparation and Mechanical Properties of Multiwalled Carbon nanotube-fiber Reinforced Vinyl Ester Composites
指導教授:馬振基馬振基引用關係
指導教授(外文):Ma, Chen-Chi M.
學位類別:碩士
校院名稱:國立清華大學
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:2012
畢業學年度:100
語文別:中文
論文頁數:270
中文關鍵詞:碳纖維玻璃纖維多壁奈米碳管乙烯酯樹脂纖維強化複合材料
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本研究旨在探討多壁奈米碳管(MWCNT)與氧化石墨烯(GO)對於玻璃纖維/乙烯酯樹脂(GF/VE)及碳纖維/乙烯酯樹脂(CF/VE)在機械強度上的影響,並比較多壁奈米碳管經不同表面改質方法後,於高分子材料中的相容性。
將P-MWCNT、TEVOS-MWCNT及Allyl-MWCNT加至玻璃纖維/乙烯酯纖維複合材料當中,玻璃纖維強化乙烯酯複合材料的拉伸強度由227.5MPa提升為254.06MPa (1phr MWCNT/GF/VE)、 258.55MPa (1phr TEVOS-MWCNT/GF/VE)與275.45MPa (1phr Allyl-MWCNT/GF/VE);玻璃纖維強化乙烯酯複合材料的破裂韌性由0.76kJ/m2,降為0.73kJ/m2 (1phr P-MWCNT/GF/VE),而改質碳管的強度分別提升為0.94kJ/m2 (1phr TEVOS-MWCNT/GF/VE)與1.07kJ/m2 (1phr Allyl-MWCNT/GF/VE),因具有官能基與樹脂有較好的界面作用力,可以提升纖維層與層之間的強度,使材料的裂縫成長速度下降,提升材料的破裂韌性。
玻璃纖維強化乙烯酯複合材料玻璃轉移溫度(Tg)由89.05oC,提升為106.78oC (1phr P-MWCNT/GF/VE)、107.70oC (1phr TEVOS-MWCNT/GF/VE)及109.70oC (1phr Allyl-MWCNT/GF/VE)。多壁奈米碳管可以阻礙材料之高分子鏈段運動, Allyl-MWCNT及TEVOS-MWCNT除了能阻斷的高分子鏈運動外,與樹脂間具有較強的界面作用力,提高纖維與樹脂之間之界面相容性,故能夠大幅提昇複合材料系統的熱穩定性。
將P-MWCNT、TEVOS-MWCNT、Allyl-MWCNT及GO加至碳纖維/乙烯酯纖維複合材料當中,碳纖維強化乙烯酯複合材料的拉伸強度由369.45MPa,提升為448.68MPa (1phr P-MWCNT/CF/VE)、465.15MPa (1phr TEVOS-MWCNT/CF/VE)、476.45MPa (1phr Allyl-MWCNT/CF/VE)及,505.04MPa(1phr GO/CF/VE),加入1phr氧化石墨烯的碳纖維強化乙烯酯複合材料有最佳強度。碳纖維複合材料的抗折強度為272.45MPa,當加入1phr P-MWCNT時,其強度會提昇至501.53MPa,而加入1phr的TEVOS-MWCNT與Allyl-MWCNT時,其強度分別為511.45MPa與521.56MPa,而最佳表現值為加入1phr氧化石墨烯,其值為558.07MPa。碳纖維強化乙烯酯複合材料的破裂韌性由0.80kJ/m2,提升為0.91kJ/m2 (1phr P-MWCNT/CF/VE)、1.04kJ/m2 (1phr TEVOS-MWCNT/CF/VE)及1.07kJ/m2 (1phr Allyl-MWCNT/CF/VE)。碳纖維強化乙烯酯複合材料玻璃轉移溫度(Tg)由98.18oC,提升為114.33oC (1phr P-MWCNT/CF/VE)、 115.67oC (1phr TEVOS-MWCNT/CF/VE)與116.67 oC (1phr Allyl-MWCNT/CF/VE)。

In this study, Multi-walled carbon nanotube(MWCNT) was modified with different methods. The Allyl-MWCNTs were prepared via free radical reaction with allylamine, which contains the ethylene groups for increase interaction between MWCNTs and vinyl ester (VE). The TEVOS was grafted on the MWCNTs surface to prepare MWCNT-TEVOS.
From the mechanical properties study, the tensile strength of glass fiber/vinyl ester was increased from 227.5MPa to 254.06MPa when 1phr P-MWCNT content was added to neat GF/VE composite. The tensile strength of GF/VE composites was increased to 258.55 MPa (with 1phr TEVOS-MWCNT) and to 275.45MPa (with 1phr Allyl-MWCNT). Modified MWCNT can improve the tensile strength of the GF/VE than that was added with unmodified MWCNT. The fracture toughness (GIC) of GF/VE composites was increased from 0.76 kJ/m2 (neat GF/VE) to 0.83kJ/m2 (with 0.25 phr MWCNT) and to 0.94 kJ/m2 (with 1.0phr TEVOS-MWCNT) and to 1.07 kJ/m2 (with 1.0phr Allyl-MWCNT). Allyl-MWCNT possesses the best interface bonding between fiber and matrix that exhibits best fracture toughness of these three kinds of composites. The Tg of GF/VE composite was 89.05℃. The GF/VE composite with 1phr TEVOS-MWCNT and Allyl-MWCNT shows the Tg which was 107.70℃, and 109.70℃ respectively. It indicated that thermal stability of composite can be improved even when a small quantity of functionalized MWCNTs was added

From the mechanical properties study, the tensile strength of carbon fiber/vinyl ester was increased from 369.45MPa to 448.68MPa when 1phr P-MWCNT content was added to neat CF/VE composite. The tensile strength of CF/VE composites increased to 465.15MPa (with 1phr TEVOS-MWCNT) and to 476.45MPa (with 1phr Allyl-MWCNT). Modified MWCNT can improve the tensile strength of the CF/VE than that of unmodified MWCNT/CF/VE composite. The GO/CF/VE composites show the best tensile strength, which were 505.04MPa with 1 phr filler content. The flexural strength of CF/VE composites was increased from 272.45MPa (neat GF/VE) to 501.53 MPa (with 1.0 phr MWCNT) and to 511.45MPa (with 1.0phr TEVOS-MWCNT) and to 521.56MPa (with 0.5phr Allyl-MWCNT).Allyl-MWCNT/CF/VE composite possesses better flexural strength than that of unmodified MWCNT/CF/VE. The GO/CF/VE composites show the best flexural strength, which was 558.07MPa with 1 phr filler content. The fracture toughness (GIC) of CF/VE composites increased from 0.80 kJ/m2 (neat CF/VE) to 0.95kJ/m2 (with 0.5 phr MWCNT) and to 1.04 kJ/m2 (with 1.0phr TEVOS-MWCNT) and to 1.07 kJ/m2 (with 1.0phr Allyl-MWCNT). Allyl-MWCNT/CF/VE exhibits the best fracture toughness due to the improvement of interface bonding between fiber and matrix. The Tg of CF/VE composite was 98.18℃. The CF/VE composite with 1phr TEVOS-MWCNT and Allyl-MWCNT shows the Tg which was 115.67℃, and 116.67℃respectively. It indicated that thermal stability of composite can be improved even when a small quantity of functionalized MWCNTs was added.

目 錄
中文摘要 I
Abstract III
謝 誌 V
目 錄 VII
圖目錄 XXVII
表目錄 XXXVII
第一章 緒 論 1
第二章 風力發電 6
2-1風力發電 6
2-2風力葉片 9
2-2-1葉片翼型 9
2-2-2葉片材料 11
2-3葉片製程[5] 13
2-4風力發電葉片生產基本要求[8] 17
2-4-1 對葉片生產商的要求[8] 17
2-4-2對風電葉片生產技術流程的要求[8] 17
2-4-3 對葉片元件之積層板的實驗測試要求[8] 18
2-4-4 疲勞要求 21
2-5結論 22
第三章 文獻回顧及理論基礎 24
3-1奈米碳管[2] 25
3-1-1奈米碳管之結構[4] 26
3-1-2奈米碳管的製備 [3, 8-15] 29
3-1-3奈米碳管的特性 33
3-1-4奈米碳管的改質 43
3-2石墨烯(GRPHENE) 54
3-2-1單層石墨烯 54
3-2-2多層奈米奈米石墨烯片(Nano Graphene Platelets, NGP) 56
3-2-3製備方法 56
3-2-4石墨烯的特性[63] 60
3-3碳纖維 63
3-3-1碳纖維的結構 63
3-3-2碳纖維的表面處理[69] 67
3-3-3碳纖維的機械性質[69] 69
3-4乙烯酯樹脂 72
3-4-1乙烯酯樹脂的特性 73
3-4-2 乙烯酯樹脂之硬化反應 77
3-4-3 乙烯酯樹脂之應用[69] 79
3-5 奈米高分子複合材料 81
3-5-1纖維複合材料 83
3-5-2混合法則 83
3-5-3Halpin and Tsai eqution 86
3-6 文獻回顧 87
3-6-1 奈米碳管/乙烯酯樹脂 87
3-6-2奈米粒子/纖維強化複合材料[86] 96
3-6-3 奈米碳管/纖維強化材料 108
3-6-3-1奈米碳管強化基材之階級複合材料 110
3-6-3-2奈米碳管強化纖維之階級複合材料 113
3-6-3-3破裂韌性(Fracture toughness) 116
3-6-4 纖維複合材料於風力葉片相關研究[112] 134
3-7結論 148
參考文獻 149
第四章 研究目的與內容 160
4-1研究目的 160
4-2研究內容 161
第五章 實驗方法 164
5-1實驗藥品 164
5-2實驗儀器設備 168
5-3 實驗流程 169
5-4 實驗步驟 170
5-4-1酸改質多壁奈米碳管(AO-MWCNT) 170
5-4-2 TEVOS改質多壁奈米碳管(TEVOS-MWCNT) 171
5-4-3自由基接枝甲基丙烯酸環氧丙酯多壁碳管(GMA-MWCNT) 171
5-4-4 Allylamine改質多壁奈米碳管(Allyl-MWCNT) 172
5-4-5氧化石墨烯(Graphene oxide, GO) 172
5-4-6多壁奈米碳管/乙烯酯樹脂複合材料之製備 173
5-4-7 多壁奈米碳管及GO/碳纖維/乙烯酯樹脂複合材料之製備 173
5-4-8 多壁奈米碳管/玻璃纖維/乙烯酯樹脂複合材料之製備 174
5-5 測試方法 175
5-5-1.結構分析 175
5-5-2.機械性質分析 175
5-5-3.型態學分析 189
5-5-4.熱性質分析 190
參考文獻 190
第六章 結果與討論 192
6-1改質奈米碳管鑑定 192
6-2多壁奈米碳管補強乙烯酯樹脂強化材料 203
6-2-1機械性質 203
6-2-2形態學 211
6-3 多壁碳管補強玻璃纖維乙烯基樹酯複合材料 213
6-3-1機械性質 213
6-3-2 形態學 223
6-3-3熱性質 227
6-4多壁奈米碳管/碳纖維複合材料 231
6-4-1機械性質 231
6-4-2 形態學 245
6-4-3熱性質 249
6-5多壁奈米碳管/玻璃纖維複合材料與碳纖維複合材料比較 252
第七章 結論 256


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第五章

1. 林瑋寧,國立清華大學化學工程系碩士論文, 2010.
2. ASTMD790-07. Standard Test Methods for Flexural Properties of Unreinforced and Reinforced Plastics and Electrical Insulating Materials.
3. ASTMD3039-00. Standard Test Method for Tensile Properties of Polymer Matrix Composite Materials.
4. ASTMD638-08. Standard Test Method for Tensile Properties of Plastics.
5. ASTMD256-06a. Standard Test Methods for Determining the Izod Pendulum Impact Resistance of Plastics.
6. ASTMD 2344/D 2344M – 00 (Reapproved 2006) Standard Test Method for Short-Beam Strength of Polymer Matrix Composite Materials and Their Laminates.
7. ATMD5045 – 99 (Reapproved 2007) Standard Test Methods for Plane-Strain Fracture Toughness and Strain Energy Release Rate of Plastic Materials.
8. Designation: D 5528 – 01 (Reapproved 2007) Standard Test Method for Mode I Interlaminar Fracture Toughness of Unidirectional Fiber-Reinforced Polymer Matrix Composites.
9. 國科會貴中儀器中心.
第六章

1. 黃彥瑋,國立清華大學化學工程系碩士論文, 2009.
2. M. Hussain, A. Nakahira and K. Niihara. Mechanical property improvement of carbon fiber reinforced epoxy composites by Al,O, filler dispersion, Materials Letters, 26, 1996, pg185-191.
3. A. Godara, L. Mezzo, F. Luizi, A. Warrier, S.V. Lomov, A.W. van Vuure, L. Gorbatikh, P. Moldenaers, I. Verpoest., Influence of carbon nanotube reinforcement on the processing and the mechanical behaviour of carbon fiber/epoxy composites., C arbon, 47, 2009, pg2914 –2923.

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