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dc.contributorJih-Mirn Jehngen_US
dc.contributor.authorLin, Wei-Chenen_US
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dc.description.abstract本研究利用Hummers-Offeman法製備出氧化石墨(GO),再成功地將氧化石墨以簡易的方式還原成單層石墨烯(XGS)。利用綠色化學法進行還原,將微量的酸性溶液與氧化石墨進行反應,去除氧化石墨上大量的含氧官能基;利用相變化的原理,水和鹽酸小分子進入氧化石墨層與層間,藉由加熱達到沸點時從液相轉變為氣相,體積大幅增加,達到脫層石墨烯並使層板部分還原,製備過程中不僅具高安全性且低污染。 探討氧化石墨與石墨烯兩系統因官能基數多寡所造成基本性質的差異。氧化石墨與雙官能基修飾分子4-isocyanato-4’(3,3-dimethyl- 2,4-dioxo-azetidino)diphenyl-methane(IDD)和親水性聚醚雙胺JEFFAMINE ED-2003反應後,氧化石墨層間距由原先7.8Å已大幅提升至脫層,生成氧化石墨烯,但透過X射線繞射觀察(XRD)仍有些微堆疊現象產生。脫層後的氧化石墨易因凡德瓦爾力再行聚集,研究中利用本實驗室開發的poly(urea/malonamide)規則性樹枝狀高分子依代數提供不同程度的立體障礙,與其進行反應,探討其堆疊現象之差異。 利用綠色還原法脫層後的單層石墨烯,同樣觀察到有些微石墨烯片有重新堆疊的現象產生,藉由雙官能基修飾分子IDD與石墨烯片上殘留的含氧官能基反應後,可使堆疊現象消失,後續再接上聚醚雙胺JEFFAMINE與規則性樹枝狀高分子亦無堆疊現象產生。從氧化石墨與石墨烯系統的研究結果顯示,藉由接枝改質可使氧化石墨達到脫層效果與大幅改善兩系統的堆疊現象。 脫層之石墨烯複合材料受限於高分子影響,電子不易傳導,因此,本研究藉由銀離子吸附在層板表面高分子進行原位還原(in-situ reduction)。奈米銀粒子於層板上還原後成為半導體,提升了電子傳遞能力,功函數數值介於4.72 – 4.76 eV之間,證明石墨烯/奈米銀粒子複合材料具有潛力應用在光電元件中的電極材料。zh_TW
dc.description.abstractExfoliated graphene sheets (XGS) were prepared from graphite oxide (GO) via a green chemistry route. Dehydration of GO is the main mechanism for the reduction and transformation of C-C bonds from sp3 to sp2. The oxygen-containing groups of GO would decompose to produce gases (H2O) and volatile substances (HCl) during the thermal treatment process. For a successful exfoliation process, the pressure generated from the evolved gases that causes rapid expansion would exceed Van der Waals forces holding GO sheets together. Different contents of the oxygen-containing moieties on the graphite oxide and graphene surface would bring about various grafting ratios of the intended compounds. First, 4-isocyanato-4’(3,3-dimethyl-2,4-dioxo- azetidino) diphenyl -methane (IDD) reacted with carboxylic acid or hydroxy functional group on the graphite oxide and graphene surface to provide a reactive site. Subsequently, a polyetheramine, JEFFAMINE® ED-2003 was reacted with the dione functional group leaving the other pendant primary amine as the grafting site for an intended dendron. The content of functional groups and the size of grafting compounds play an important role in keeping graphene and graphene oxide from aggregation. Via the thermal treatment process, XGS comprised randomly ordered graphitic platelets in a corrugated structure. As the IDD molecules reacted with the reduced graphene sheets, the spacings of graphene single-layers could be well maintained. As for GO, the covalent attachment of JEFFAMINE ED-2003 was required to achieve exfoliation. We demonstrated that the respective grafting of relatively low molecular weight JEFFAMINE ED-2003 to GO, and IDD to the reduced graphene was sufficient to prevent single-layers from aggregation. Due to poor electronic transfer ability of the polymers attached to the exfoliated graphene hybrids, silver nanoparticles were adsorbed on the grafted polymers to increase the conductivity. The work functions of XGS/Ag nanohybrids were measured to be 4.72 – 4.76 eV. The large work functions suggest that these XGS/Ag nanohybrids can potentially be applied as electrode materials for optoelectronic devices.en_US
dc.description.tableofcontents中文摘要 I ABSTRACT II 目錄 IV 表目錄 VI 圖目錄 VII 代號說明 X 第一章、緒論 1 1.1 碳材之簡介 1 1.2 高分子之簡介 2 第二章、文獻回顧與研究動機 4 2.1 石墨烯(GRAPHENE)之簡介 4 2.1.1 石墨烯之發展 4 2.1.2 石墨烯(graphene)之製備方法 7 2.1.3 氧化石墨 (graphite oxide, GO)之製備方法 20 2.1.4 石墨烯之應用 21 2.2 規則樹枝狀分子(DENDRIMER)簡介 29 2.2.1 Dendrimer合成路徑 31 2.2.2 Dendrimer結構與特性 32 2.2.3 Dendrimer與線性高分子比較 34 2.2.4 規則樹枝狀衍生物 35 2.3 研究動機 36 第三章、實驗內容 37 3.1 藥品及溶劑部分 37 3.2 實驗儀器 40 3.3 實驗步驟 42 3.3.1 氧化石墨之製備 42 3.3.2 IDD之製備 44 3.3.3 Poly(urea/malonamide) dendrimer之製備 46 3.3.4 單層片狀石墨烯之製備 48 3.3.5 單層氧化石墨烯/金屬銀複合材料之製備 49 3.3.6 單層石墨烯/金屬銀複合材料之製備 52 第四章、 實驗內容 55 4.1 DENDRON的合成與鑑定 55 4.1.1 反應選擇性單體IDD之合成與鑑定 55 4.1.2 C18系列收斂式poly(urethane/malonamide) dendron 之合成與鑑定 60 4.2 氧化石墨與脫層石墨烯的鑑定與特性分析 72 4.2.1 傅立葉式紅外線光譜儀(FT-IR) 75 4.2.2 廣角X光繞射分析儀(WXRD) 76 4.2.3 元素分析(Elemental Analyzer,EA) 78 4.2.4 熱重損失分析儀 ( thermogravimetric analyzer)(TGA) 79 4.2.5 化學分析電子儀分析 80 4.2.6 拉曼散射光譜儀 85 4.3 網狀單層氧化石墨烯複合材料之合成與鑑定 88 4.3.1 廣角X光繞射分析儀 (wide angle x-ray diffraction)(WXRD) 93 4.3.2 穿透式電子顯微鏡 (transmitting electron microscope)(TEM) 與 Selected area electron diffraction pattern(SAED) 95 4.3.3 網狀單層氧化石墨烯複合材料之脫層機制 99 4.4 網狀單層石墨烯複合材料之合成與鑑定 100 4.4.1 廣角X光繞射分析儀 (wide angle x-ray diffraction)(WXRD) 106 4.4.2 穿透式電子顯微鏡 (transmitting electron microscope)(TEM) 與 Selected area electron diffraction pattern(SAED) 108 4.4.3 網狀單層石墨烯複合材料之脫層機制 113 4.5 金屬銀混成材料之合成與鑑定 114 4.5.1網狀氧化石墨烯/金屬銀混成材料之合成與鑑定 114 4.5.2網狀石墨烯/金屬銀混成材料之合成與鑑定 121 第五章、結論 123 第六章、參考文獻 125 第七章、附錄 132zh_TW
dc.subjectgraphite oxideen_US
dc.subjectsilver nanoparticleen_US
dc.titleSynthesis and Application of Network Single-layered Graphene/Ag Hybridsen_US
dc.typeThesis and Dissertationzh_TW
item.fulltextno fulltext-
item.openairetypeThesis and Dissertation-
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