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研究生： Juwita Herlina Riskawati
Juwita Herlina Riskawati
論文名稱： Characterization of Fluorocarbon Incorporated Graphene Composite Towards Oxygen Doping
Characterization of Fluorocarbon Incorporated Graphene Composite Towards Oxygen Doping
指導教授： 今榮東洋子
Toyoko Imae
口試委員: 氏原真樹
Masaki Ujihara
鄭智嘉
Chih Chia Cheng
學位類別： 碩士
Master
系所名稱： 應用科技學院 - 應用科技研究所
Graduate Institute of Applied Science and Technology
論文出版年： 2018
畢業學年度： 106
語文別： 英文
論文頁數： 95
中文關鍵詞： Graphene Composite 、Fluorocarbon 、Oxygen Doping 、Graphene Oxide 、Generation 4 (OH) PAMAM Dendrimer 、Pentafluoropropionic Acid
外文關鍵詞： Graphene Composite, Fluorocarbon, Oxygen Doping, Graphene Oxide, Generation 4 (OH) PAMAM Dendrimer, Pentafluoropropionic Acid
相關次數： 點閱：409  下載：1 
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    • 摘要

    碳氟摻雜石墨烯複合材料應用於生物醫學方面尚未被廣泛探索。在本研究中我們使用具有奈米尺寸的氧化石墨烯(graphene oxide, NGO)、具羥基(-OH)的聚（酰氨基）胺樹枝狀聚合物（OH-terminated poly (amido) amine dendrimer, Den-OH）、五氟丙酸(pentafluoropropionic acid)和氟化聚乙二醇(fluorinated polyethylene glycol, F10H5COOPEG5000)製備出具摻雜碳氟化合物的石墨烯複合材料(NGO/Den(OH)-F)。NGO/Den(OH)-F因藉由F10H5COOPEG5000進行表面官能化進而對其溶解度產生影響。
    氧化石墨烯的保留氧氣的實驗(oxygen retention experiment)顯示出，氧化程度少的氧化石墨烯(GO(1))比氧化程度高的氧化石墨烯具有更好的保留氧氣的能力。同理在GO-F10H5COOPEG5000複合物上也觀察到類似地保留氧氣的趨勢即與氧化程度少的氧化石墨烯-F10H5COOPEG5000複合物比氧化程度高的氧化石墨烯-F10H5COOPEG5000複合物具有更好的保留氧氣的能力。
    然而，GO-F10H5COOPEG5000複合物比只有氧化石墨烯約高出四倍的保留氧氣的能力。由實驗結果我們假設此複合物在氟化區域的保留氧氣因透過范德華相互作用(Van der Waals interaction)使氧化石墨烯上的氧氣吸附更有效。這些實驗結果顯示出F10H5COOPEG5000摻雜GO的複合物可當作氧氣載體材料並應用在活性氧治療(active oxygen therapy)中。

    Abstract

    Biomedical applications of fluorocarbon incorporated-graphene composite remain unexplored and widely opened. Fluorocarbon incorporated- graphene composite was prepared from nano-sized graphene oxide (NGO), OH-terminated poly (amido) amine dendrimer (Den-OH), pentafluoropropionic acid, and fluorinated polyethylene glycol (F_10 H_5 COOPEG_5000). Surface functionalization of NGO/Den(OH)-F by F_10 H_5 COOPEG_5000 gave impact on its solubility.
    The oxygen retention experiment of graphene oxide showed that the less- oxidized graphene oxide (GO (1)) had better ability in retaining oxygen compared to the highly-oxidized graphene oxide. Similar oxygen retention tendency was observed even on the GO -F_10 H_5 COOPEG_5000 complex: The less-oxidized graphene oxide-F_10 H_5 COOPEG_5000 complex had better ability on oxygen retention than the highly-oxidized graphene oxide-F_10 H_5 COOPEG_5000 complex.
    However, the oxygen retention ability of GO -F_10 H_5 COOPEG_5000 complex was about four times higher than that of graphene oxide alone. It should be assumed that the oxygen retention on the fluorinated domains in the complex should be more effective than the oxygen adsorption on oxidized graphene by Van der Waals interaction. These results indicate the F_10 H_5 COOPEG_5000 incorporated graphene oxide (GO) complex can be used as an oxygen-carrier material for active oxygen therapy.

    Table of Content Abstract………………………………………………………………………..,,,,,,,i 摘要……………………………………………………………………………….ii Acknowledgement.……………………………………………………………….iii Table of Content………………………………………………………………..,,,,iv List of Figures…………………………………………………………………......ix List of Tables…………………………………………………………………….xiv Chapter I. General Introduction……………………………………………………1 I. 1. Introduction………………..………………………………………………………..1 I. 1. 1. Graphite Flake………..…………….………………….……………….……1 I. 1. 2. Graphene…….………...………………………………….……………….…2 I. 1. 3. Graphene Oxide….….…......………………..…………….…………….….3 I. 1. 4. G4-(OH)-PAMAM Dendrimer….....……..……….…….….…………….4 I. 1. 5. Pentafluoropropionic Acid.…………….……………….…..…………….4 I. 1. 6. Fluorinated Polyethylene Glycol Derivative……...…..….…………….5 I. 1. 7. N,N’-Dicyclohexylcarbodiimide (DCC)…....…...….…...………...…...6 I. 1. 8. 4-Dimethylaminopyridine (DMAP)…........….……..……...………......6 I. 1. 9. Nano-Composite……….….……………………..………..……..………..7 I. 1. 10. Active Oxygen Therapy.……….………….……………..…..…….……..7 I. 1. 11. Adsorption-Desorption.….…………………………….….………..…....8 I. 2. Objective of The Work…..…………...……………………………………...9 Chapter II. Experimental Section………………………………………………..11 II. 1. Materials……………………………………………………………………11 II. 2. Instruments..…………..……………………………………………………12 v II. 3. Methods…….………………………………………………………………13 II. 3. 1. Preparation of The Nano-Graphene Oxide (NGO) Colloidal Suspension from Commercial Aqueous Graphene Oxide…...…….13 II. 3. 2. Synthesis of The NGO/Den (OH)-F Composite….…………….….14 II. 3. 3. Preparation of The [NGO/Den (OH)]-?10?5??????5000 Mixture……………………………………………………………...18 II. 3. 4. Preparation of The Less Oxidized Graphene Oxide [GO (1)] with Average Particle Size Less than 200 nm from Graphite Flake 4 μm Size…........................................................................................19 II. 3. 5. Preparation of The More Oxidized Graphene Oxide [GO (2)] with Average Particle Size Less Than 200 nm from Graphite Flake 4 μm Size….………...………….……...…………..………………..25 II. 3. 6. Preparation of The [GO (1]-?10?5??????5000 Mixture………...29 II. 3. 7. Preparation of The [GO (2)]- ?10?5??????5000 Mixture…….…31 II. 3. 8. Oxygen Adsorption-Desorption Experiment of The Less Oxidized Graphene Oxide [GO (1)], The More Oxidized Graphene Oxide [GO (2)], The [GO (1)-?10?5??????5000], The [GO (2)- ?10?5??????5000] by Using Thermo Gravimetric Analysis…….32 II. 3. 9. Thermal Decomposition of The Graphite Flake, The Less Oxidized Graphene Oxide [GO (1)], and The More Oxidized Graphene Oxide [GO (2)] by Using Thermo Gravimetric Analysis…......…...….......33 Chapter III. Results and Discussion……………………………………………....34 III. 1. Preparation of The Nano-Graphene Oxide [NGO], The NGO/Den(OH)-F Composite, and The Mixture of [NGO/Den (OH)-F]-F10H5COOPEG5000…34 III. 1. 1. Preparation of The Nano-Graphene Oxide Colloidal Suspension vi from Commercial Aqueous Graphene Oxide………………...….34 III. I. 2. Preparation of The NGO/Den (OH)-F Composite……………..…35 III.1. 3. Preparation of The ?10?5 ???5000……………………………...37 III.1.4. Preparation of The NGO/Den (OH)-F Composite and ?10?5 ???5000 Mixture…………………………………………38 III. 2. Characterization of The Nano-Graphene Oxide [NGO], The NGO/Den (OH)-F Composite, and The Mixture of [NGO/Den (OH)-F]-F10H5COOPEG5000……………………..……………39 III. 2. 1. Characterization of The Nano-Graphene Oxide from Commercial Aqueous Graphene Oxide…….......…………….………………......39 III. 2. 2. Characterization of The NGO/Den (OH)-F Composite Chemical Composition by Using FTIR Instrument……...……………..…..43 III. 2. 3. Characterization The Nano-Graphene Oxide [NGO], [NGO/Den (OH)-F]- ?10?5 ???5000, and NGO/Den (OH)-F Mixed With ?10?5 ???5000 Morphologies by Using Transmission Electron Microscopy……...………………………………..……...45 III. 2 .4. Characterization of The Nano-Graphene Oxide [NGO] and NGO/Den (OH)-F Morphologies by Using Atomic Force Microscopy…………………………….…………………..…….46 III. 2. 5. Characterization of The Nano-Graphene Oxide (NGO), NGO/Den (OH)-F, and NGO/Den (OH)-F Mixed with ?10?5 ???5000 Average Particle Sizes and Zeta Potential Values at Variety of pH……………….………………………………...49 III. 2. 6. Characterization of ?ℎ? ?10?5??????5000 ???????? ???? ....57 III. 3. Preparation of The Less Oxidized Graphene Oxide [GO (1)] and The More vii Oxidized Graphene Oxide [GO (2)] from Graphite Flake (4 μm Diameter Size)…………………………………………………………………......58 III. 3. 1. Preparation of The Less Oxidized Graphene Oxide [GO (1)]….58 III. 3. 2. Preparation of The More Oxidized Graphene Oxide [GO (2)]…60 III. 4. Characterization of The Less Oxidized Graphene Oxide [GO (1)], The More Oxidized Graphene Oxide [GO (2)], The GO (1) Coated with F10H5 PEG5000, and The GO (2) Coated with F10H5 PEG5000……..……..62 III. 4. 1. Characterization of The Less Oxidize Graphene Oxide [GO (1)] and The More Oxidized Graphene Oxide [GO (2)]Particle Sizes..62 III. 4. 2. Characterization of The Less Oxidize Graphene Oxide [GO (1)], The More Oxidized Graphene Oxide [GO (2)], The [GO (1)-?10?5??????5000]and The [GO (2)- ?10?5??????5000] Morphologies by Using Transmission Electron Microscopy……………………………………...……..65 III. 4. 3. Characterization of The Graphite Flake, The Less Oxidized Graphene Oxide [GO (1)] and The More Oxidized Graphene Oxide [GO (2)] Chemical Composition by Using FTIR Spectroscopy….67 III. 4. 4. XRD Analysis of The Graphite Flake, The Less Oxidized Graphene Oxide [GO (1)] and The More Oxidized Graphene Oxide [GO (2)]………………………………………………………....68 III. 4. 5. Themal Decomposition of The Graphite Flake, The Less Oxidized Graphene Oxide [GO (1)], and The More Oxidized Graphene Oxide[GO (2)] by Using Thermo Gravimetric Analysis…..………70 III. 5. Oxygen Adsorption-Desorption Behavior of The Less Oxidized Graphene Oxide [GO (1)], The More Oxidized Graphene Oxide [GO (2)], The viii GO (1) Coated with F10H5 PEG5000, and The GO (2) Coated with F10H5 PEG5000……………………………………………………………72 III. 6. Graph of Oxygen Adsorption-Desorption of The Less Oxidized Graphene Oxide [GO (1)], The More Oxidized Graphene Oxide [GO (2)], The [GO (1) -F10H5 PEG5000] ,and [GO (2) −F10H5 PEG5000]…………………81 III. 7. Nitrogen Adsorption Ability of The [GO (1) - F10H5 PEG5000] as Confirmation of Oxygen Adsorption Characteristic of The Mixture of GO-F10H5 PEG5000 …………………………………………………........85 Chapter IV. Conclusion………………………………………………………......88 Reference………………………………………………………………………....90

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