在傳統的積層複合材料中，破壞往往與基材的損傷、界面鍵結、纖維本身強度以及層間剪強度脫不了關係，當複合材料破壞時，往往有兩個以上的破壞因素存在於複合材料中，本研究針對添加奈米碳材之複合材料受力時造成的破壞行為與破壞因素對機械性質的關聯性進行探討。首先將天然石墨利用哈默法(Hummers’ method)製備氧化石墨後分別以熱膨脹剝離與液相剝離法製備氧化石墨微片，對產物進行分析檢測比較後導入纖維強化複合材料中，並與Angstron Materials, Inc.所生產的石墨烯進行抗折強度、模數、層間剪強度等機械性質的比較，觀察兩者的微觀影像，分析複合材料的破壞與強化機制，並與添加奈米碳管之纖維強化複合材料比較機械性質與破壞強化機制，最後利用奈米碳材/環氧樹脂兩相複合材料觀察石墨烯或氧化石墨烯與環氧基材的相互影響。
實驗結果顯示，以熱剝離法與液相製備法皆能將氧化石墨製備為更薄的微片(分別稱為H-GONP及L-GONP)，製備結果各有優劣，以熱剝離法製備會令表面無含氧官能基，而以液相剝離法容易有界面活性劑殘留，不使用界面活性劑難以將氧化石墨剝離成更薄的氧化石墨微片。在複合材料檢測結果中，三相複合材料的三點抗折強度僅在添加0.5 wt%石墨烯於丙酮中超音波震盪所製備的環氧基複合材料的結果較佳，其抗折強度提升了18 %，添加自製的H-GONP與L-GONP則無法達到預期效果，前者是由於添加物團聚，後者則是在基材與纖維間的裂縫成長、添加物本身的界面鍵結等諸多因素相互影響下所致。而添加0.5 wt%的添加物製備兩相環氧樹脂複合材料的三點抗折結果以及利用短樑試驗檢測層間剪強度皆無顯著改變。利用SEM對兩相複合材料、三相複合材料以及短樑試驗的破斷面進行微觀分析，剖析複合材料中不同的破壞行為所造成的破壞形貌，並探討石墨烯與氧化石墨微片在複合材料中的影響。

The damage in the conventional laminated composites were related with the defect of matrix, the interfacial bond, the strength of fiber and the interlaminar shear strength. Two or more factors were often observed when the laminated composites fracture. In this study, we investigated the fracture behaviors and their relationship with the mechanical properties for the laminated composites with the addition of carbon nanofillers. Two types of graphene oxide nanoplatelets (GONPs), produced using liquid-phase exfoliation in surfactant/water solution and using thermal exfoliation from the graphite oxide by Hummers’ method using the natural graphite, and one commercially available graphene nanoplatelet (GNP) from Angstron Materials, Inc. were used as the carbon nanofillers. The flexural properties and the interlaminar shear strength (ILSS) of the composites were measured, the fracture surfaces were observed, and the fracture behavior and mechanisms were analyzed, which were also compared with these of composites with carbon nanotube addition. In addition to carbon nanofiller/carbon fiber/epoxy three-phase composites, the fracture behavior of carbon nanofiller/epoxy two-phase composites was studied to further elucidate the interaction between carbon nanofiller and epoxy matrix.
Experimental results indicated that the thinner GONPs can be produced from the graphite oxide using both thermal exfoliation (called H-GONP) and liquid exfoliation (called L-GONP). However, the oxygen functional group will be removed using thermal exfoliation, and the surfactant will remain in the L-GONP using liquid exfoliation. Flexural strength measurements showed an 18% increase for a 0.5 wt% GNP addition in three-phase composites. However, no strength enhancement was found when H-GONPs and L-GONPs were adopted. The reasons were attributed to the aggregation of H-GONPs, and to the interaction among carbon fibers, carbon nanofillers and the epoxy matrix when L-GONPs were used. No obvious change in the ILSS was also measured. For the two-phase composites with an addition of 0.5 wt% GNP, the flexural strength also remained relatively constant. The fracture surfaces of both two-phase and three-phase composites after both flexural tests and short beam shear tests were observed using FE-SEM, and the fracture behavior and mechanisms were discussed.

中文摘要 I
Abstract III
主目錄 V
表目錄 IX
圖目錄 X
第一章 緒論 1
1.1 前言 1
1.2 研究目的 2
第二章 文獻回顧 3
2.1石墨烯 3
2.1.1簡述石墨烯 3
2.1.2石墨烯的製造方法 4
2.1.2.1 Bottom-Up Graphene Processes 4
2.1.2.2 Top-Down Graphene Processes 5
2.1.2.2.1 純石墨類製造 5
2.1.2.2.2 石墨衍生物製造 6
2.2強化材 14
2.3基材 16
2.3.1酚醛樹脂 17
2.3.2環氧樹脂 17
2.4複合材料的破壞與強化機制 24
2.5石墨烯強化高分子基複合材料 28
2.6石墨烯/碳纖維強化高分子基複合材料 40
第三章 實驗材料、方法與步驟 46
3.1氧化石墨微片製備 46
3.1.1實驗材料與設備 46
3.1.2實驗步驟 46
3.1.2.1氧化石墨製備 46
3.1.2.2液相製備 46
3.1.2.3熱剝離製備 47
3.2複合材料製備 49
3.2.1實驗材料與設備 49
3.2.2實驗步驟 52
3.2.2.1奈米碳材/碳纖維/酚醛基複合材料製作程序 52
3.2.2.2奈米碳材/碳纖維/環氧基複合材料製作程序 52
3.2.2.3奈米碳材/環氧基複合材料製作程序 53
3.3實驗參數 56
3.4性質測試 58
3.4.1 X-ray Diffracation分析 58
3.4.2重量損失率量測 58
3.4.3傅利葉紅外線光譜(FT-IR)分析 58
3.4.4原子力顯微鏡(AFM)分析 59
3.4.5三點抗折強度與模數 60
3.4.6短樑測試 61
3.4.7場發射掃描式電子顯微鏡(FE-SEM)觀測 61
3.4.8粒徑分析 62
第四章 結果與討論 63
4.1氧化石墨微片製備 63
4.1.1低溫氧化區段對氧化石墨影響 63
4.1.2液相製備氧化石墨微片 65
4.1.3熱剝離製備氧化石墨微片 66
4.1.3.1重量損失 66
4.1.3.2 XRD分析 67
4.1.3.3 FT-IR分析 68
4.1.3.4 AFM分析 68
4.1.3.5 SEM分析 69
4.2碳纖維強化高分子基複合材料 78
4.2.1奈米碳材/碳纖維/酚醛基複合材料之抗折強度與模數 78
4.2.2奈米碳材/碳纖維/環氧基複合材料之抗折強度與模數 79
4.2.2.1利用混拌法製備 79
4.2.2.2利用超音波震盪法製備 81
4.2.3添加奈米碳材料的破壞與強化機制 85
4.2.4環氧基複合材料之短樑試驗 107
4.3高分子基複合材料 114
4.3.1奈米碳材料/環氧樹脂複合材料三點抗折試驗 114
4.3.2奈米碳材料/環氧樹脂複合材料分散性與破壞機制 115
4.3.2.1純相環氧樹脂 115
4.3.2.石墨烯/環氧樹脂複合材料 116
4.3.3氧化石墨微片/環氧樹脂複合材料 119
第五章 結論 126
參考文獻 128

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