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研究生： 范保超
Yakub - Fam
論文名稱： 羥磷灰石-樹枝狀高分子-鉑金之奈米複合材料之製備及其應用
Fabrication of Hydroxyapatite-Dendrimer-Platinum Nanocomposites and Their Application
指導教授： 今榮東洋子
Toyoko Imae
氏原真樹
Masaki Ujihara
口試委員: 洪儒生
Lu-Sheng Hong
陳良益
Liang-Yih Chen
蔡協致
Hsieh-Chih Tsai
學位類別： 碩士
Master
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2013
畢業學年度： 101
語文別： 英文
論文頁數： 112
中文關鍵詞： 奈米複合材料 、羥磷灰石 、鉑金 、甲醛 、觸媒 、分析
外文關鍵詞： nanocomposites, hydroxyapatite, platinum, formaldehyde, catalyst, analysis
相關次數： 點閱：571  下載：6 
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  •  上一筆

    • 近年來由於奈米技術之進展使得納米複合材料被廣泛的使用在多種應用層面上，本研究製備了羥磷灰石-樹枝狀高分子-鉑金之奈米複合材料之及其在汙染物降解之探討，首先於具胺基之聚乙二胺樹枝狀高分子還原鉑金粒子，樹枝狀高分子扮演了安定劑之腳色，並以鉑金金屬離子作為鉑金前驅物，維持鉑金與胺基之莫爾比例0.2比1後添加硼氫化鈉還原劑，鉑金/樹枝狀高分子近一步藉由電性及氫鍵作用力與羥磷灰石之磷酸離子作用，並處與鈣離子與磷酸離子間，而後用水熱法及鍛燒製備出粉末態之羥磷灰石/樹枝狀高分子/鉑金之奈米複合材料，實驗發現pH之調控將影響鉑金/樹枝狀高分子與磷酸之作用力，並改變此複合材料型態。

    本研究另一部分為利用上述複合材料探討甲醛之降解，並探討不同參數下降解動力學，參數設定為攪拌速度、空氣體積、觸媒種類及數量、甲醛之濃度、鉑金之含量及溫度，此降解反應控制在一大氣壓下，以空氣中的氧氣扮演氧化劑之角色，而溶液中HCHO之殘餘濃度則利用乙酰丙酮比色法來偵測之，此分析法證實有效加速甲醛分解之最佳化條件為:攪拌效應、空氣體積225mL、甲醛與複合型觸媒之質量比1:2、初始甲醛濃度1000 ppm、pH為4情況下所製備之奈米複合材料、反應溫度為75℃，此分析法亦證實此甲醛分解轉換成二氧化碳及水蒸氣取決於甲醛於觸媒表面吸附性，而影響此吸附特性為觸媒之孔洞體積。

    Nanocomposites have been widely used in a variety of applications due to the recent advancement in nanotechnology. The fabrication of hydroxyapatite-dendrimer-platinum (HAp-DEN(PtNP)s) nanocomposites and their catalytic application on degradation of a pollutant are reported in this work. It begins with a synthesis of Pt nanoparticles (PtNP) in the presence of an NH2-terminated fourth generation poly(amido-amine) Dendrimer (DEN) as a stabilizer and PtCl62- in Pt precursors (Na2PtCl6•6H2O) at a specific molar ratio (Pt : NH2 = 0.2 : 1). The reduction of Pt complex ions was carried out by means of a reducing agent (NaBH4) at different molar ratios of NaBH4 : Na2PtCl6•6H2O. Subsequently, PtNP protected by DEN (DEN(PtNP)s) were taken in the hydroxyapatite (HAp) matrices through an electrostatic/hydrogen-bond intereaction with phosphate (PO43-) precursors of HAp and then successively between PO43- and calcium (Ca2+) precursors of HAp. The growth of HAp-DEN(PtNP)s nanocomposite was promoted by a hydrothermal synthesis at 150 oC for 15 h and turned into powders afterward. The effective condition on fabrication of HAp-DEN(PtNP)s nanocomposites was molar ratio of NaBH4 : Na2PtCl6•6H2O = 10 : 1, stirring time of 3 h, and mole ratio of NH2 : PO43- = 1 : 1. The pH adjustment (pH 12, 8, and 4) during the mixing process between DEN(PtNP)s nanoparticles and PO43- precursors affected the particular structural characteristics of HAp matrices and the distribution of DEN(PtNP)s nanoparticles in the resulting nanocomposites.

    The degradation of one of pollutants, formaldehyde (HCHO), by means of HAp-DEN(PtNP)s nanocomposite powders as a catalyst with a range of experimental variations, such as stirring, air volume, amount and type of catalyst, concentration of HCHO, pH, Pt-content and temperature. The reaction was performed at an atmospheric pressure with oxygen from an open air as an oxidant, and the remaining concentration of HCHO in the solution was detected by means of an acetylacetone colorimetric method. The analytical results elucidated that stirring effect, air volume of 225 mL, mass ratio of HCHO : catalyst = 1 : 2, HAp-DEN(PtNP)s catalyst, intial HCHO concentration of 1000 ppm, nanocomposite at pH 4, mole ratio of NH2 : PO43- = 1 : 0.3, and temperature of 75 oC effectively improved the acceleration on the oxidation rate of HCHO. The results were also supported by the reaction-rate analysis and the experimental activation energy (Ea) values at different pH of the nanocomposites. The analysis indicated that the complete oxidation process of HCHO to become carbon dioxide and water vapor relied on the adsorption process of HCHO to the catalyst.

    Cover Page (Title Page) Master's Thesis Recommendation Form Thesis Qualification Form Abstract 摘要 Acknowledgements Table of Contents List of Figures List of Tables Part A: Fabrication of Hydroxyapatite-Dendrimer-Platinum Nanocomposites Chapter I Introduction I.1. Background I.2. Problems Formulation I.3. Research Purposes Chapter II Research Methodology II.1. Research Design II.2. Materials II.3. Experimental Procedure II.3.1. Synthesis of DEN(PtNP)s nanoparticles II.3.2. Synthesis of HAp-DEN(PtNP)s nanocomposites II.3.3. Characterization Chapter III Results III.1. Fabrication of DEN(PtNP)s nanoparticles III.2. Fabrication of HAp-DEN(PtNP)s nanocomposites III.2.1. Effect of NaBH4 : Na2PtCl6.6H2O molar ratio III.2.2. Effect of stirring time III.2.3. Effect of NH2 : PO43- mole ratio III.3. The effect of pH on fabrication of HAp-DEN(PtNP)s nanocomposites III.3.1. Crystal morphology and distribution of PtNP in HAp matrices III.3.2. Functional groups and DEN content in the nanocomposites III.3.3. Crystal phase of HAp and Pt content in HAp matrices III.3.4. Quantitative results of DEN and Pt contents in the nanocomposites III.3.5. Crystal structure of HAp and Pt in the nanocomposites III.3.6. Ordering and arrangement of pores in the nanocomposites III.3.7. Surface area and pore size distribution in the nanocomposites Chapter IV Discussion IV.1. Characteristics of DEN(PtNP)s nanoparticles IV.2. Characteristics of HAp-DEN(PtNP)s nanocomposites Chapter V Conclusions Part B: Oxidation of Formaldehyde by HAp-DEN(PtNP)s Nanocomposites Chapter I Introduction I.1. Background I.2. Problems Formulation I.3. Research Purposes Chapter II Research Methodology II.1. Research Design II.2. Materials II.3. Experimental Procedure II.3.1. Preparation of colorimetric agent (CA) II.3.2. Determination of an appropriate wavelength number for formaldehyde II.3.3. Formation of a standard calibration curve for formaldehyde II.3.4. Catalytic oxidation of formaldehyde Chapter III Results III.1. Determination of a standard calibration curve for a quantification of formaldehyde III.2. Catalytic oxidation of formaldehyde III.2.1. Effect of stirring on reaction rate III.2.2. Effect of air amount on reaction rate III.2.3. Effect of catalyst amount on reaction rate III.2.4. Effect of catalyst material on reaction rate III.2.5. Effect of catalyst at different pH on the reaction rate III.3.2. Functional groups and DEN content in the nanocomposites III.2.6. Effect of NH2 : PO43- mole ratio on reaction rate III.2.7. Effect of HCHO concentration on reaction rate III.2.8. Effect of temperature on reaction rate Chapter IV Discussion IV.1. Quantitative determination of formaldehyde IV.2. Oxidation of formaldehyde Chapter V Conclusions General Conclusions Bibliography Appendix A.1. Effect of burning on HAp’s crystal structures B.1. Effect of catalyst material on HCHO decomposition B.2. Effect of stirring speed and catalyst size on HCHO decomposition B.3. Effect of temperature on HCHO decomposition Authorization Form

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