臺灣博碩士論文加值系統

本研究合成出奈米級四氧化三鐵並與silicalite-1結合成複合材料，以血紅蛋白溶液的吸附了解其吸附行為。先以四種不同的四氧化三鐵製備方法，選出在水中分散效果最佳的，進行silicalite-1的合成，以XRD確認合成出的材料為四氧化三鐵，以TEM觀察其粒徑，並由VSM觀察四氧化三鐵的飽和磁化量及矯頑力。Silicalite-1是由溶膠-凝膠法合成出沸石前驅物，再經由熟化步驟成核，最後以水熱法長晶。四氧化三鐵在熟化前、熟化後、水熱法後加入至silicalite-1前驅物中，並改變四氧化三鐵︰silicalite-1比例為1︰3、1︰1、3︰1，以XRD觀察複合材料的結晶狀況，TEM觀察複合材料中四氧化三鐵的分佈位置，選出最佳條件的複合材料進行血紅蛋白吸附實驗。合成出的材料在溶液中可經由外加磁場加以回收，且經由VSM可確認為超順磁材料。血紅蛋白吸附實驗透過改變不同的血紅蛋白濃度，以求出複合材料的飽和吸附量，與文獻值相較，本實驗所合成出的複合材料飽和吸附量為178.03 mg/g，與文獻值148 mg/g相較高出許多。最後以Langmuir方程式模擬血紅蛋白吸附行為，得到參數證明為單層的物理吸附現象。

Zeolites, microporous crystalline silicates and aluminosilicates were found to be efficient heterogeneous catalyst . The decrease of zeolite crystal size to naoscale not only brings a large surface area for the interaction to the macromolecules but also makes the uniform and to the micrometer-sized ones, nanosized zeolites become more promising candidates for a variety of nonconventional applications, especially in bio-related fields. The present work aims at preparing zeolite nanocrystals combined with magnetite (Fe3O4) nanoparticles. In this work, a facile method for the rapid synthesis of zeolite nanocrystals combined with superparamagnetic magnetite nanoparticles is described. Four different methods for preparing magnetite nanocrystals are compared. The best materials, is fully-dispersible in water, which is used for making nanocomposite with zeolite nanocrystals and discussed here. In order to facilitate the mixing of nanoparticles, we have prepared hydrophilic nanocrystals of both zeolite and magnetite. The method described in the literature [1] was followed for the preparation of magnetite and silicalite-1 [2] nanoparticles. In a typical procedure, the silicalite-1/magnetite nanocomposite was prepared by mixing of hydrophilic silicalite-1 nanoparticles and magnetite nanoparticles followed by ageing (80˚C for 6 hrs) high temperature (175˚C for 6 hrs) hydrothermal method. The product was centrifuged at 6000 rpm or collected by using external magnetic field to extract the solids. The product was characterized for their structure by XRD, SEM, TEM, BET and the magnetic properties were investigated by vibrating sample magnetometry (VSM). The phase purity of the nanocomposite was confirmed using XRD. The broadening of the peaks is attributed to the small size of the nanocrystals. The particle size of zeolite nanocrystals combined with magnetite nanoparticles is in the range of 100 nm. Hysteresis of the magnetite nanoparticle was very small, indicating superparamagnetic behavior. The saturation magnetization of magnetite particles is 31emu/g at room temperature, which is smaller than that of bulk magnetite (90 emu/g) due to surface effect. Also, the saturation magnetization of silicalite-1/magnetite nanocomposite is 7 emu/g at room temperature, which is smaller than that of silicalite-1/magnetite nanocomposite (8.9 emu/g) reported in the literature. To study whether the nanocomposite would influence the interaction between zeolite nanocrystals and biomolecules, a hemoglobin adsorption experiment was carried out. It was found that the saturated adsorption amount of hemoglobin over the nanocomposite at pH 7.0 was 178.03 mg/g, which is higher than reported in the literature (148 mg/g) indicating that the nanocomposites have a reasonable adsorption capacity for biomolecules. A key factor for fabricating small magnetically separable nanozeolites crystals is the hydrophilic nature of the nanoparticles. The method presented here produces a target material of uniform sized and superparamagnetic behavior is suitable for bioapplications.

摘要 i
ABSTRACT ii
誌謝 iv
目錄 v
圖目錄 viii
表目錄 x
第一章 前言 1
1.1 前言 1
1.2 文獻回顧 1
1.2.1 奈米氧化鐵合成 1
1.2.2 磁性奈米粒子的應用 2
1.2.3 磁性多孔材料之應用 3
1.3 研究目的 6
第二章 原理 7
2.1 沸石 7
2.1.1 沸石合成 7
2.1.2 沸石簡介 7
2.2 四氧化三鐵簡介 9
2.3 磁性簡介及磁滯曲線 11
2.4 磁性材料於生醫方面的應用 12
2.5 血紅蛋白 14
2.6 吸附現象 15
2.6.1 固液吸附 15
2.6.2 吸附模式 16
第三章 實驗 18
3.1 藥品 18
3.2 儀器 19
3.3 實驗步驟 20
3.3.1 方法一之奈米四氧化三鐵 20
3.3.2 方法二之奈米四氧化三鐵 22
3.3.3 方法三之奈米四氧化三鐵 22
3.3.4 方法四之奈米四氧化三鐵 23
3.3.5 奈米四氧化三鐵粒子與沸石silicalite-1複合材料的合成 24
3.4 血紅蛋白的吸附 26
3.4.1 血紅蛋白的吸附檢量線 26
3.4.2 血紅蛋白的吸附 26
3.5 實驗設計 27
3.5.1 不同四氧化三鐵的製備 27
3.5.2 四氧化三鐵︰silicalite-1改變的實驗規劃 27
3.5.3 血紅蛋白的吸附實驗設計 28
第四章 結果與討論 29
4.1 四氧化三鐵 29
4.1.1 四氧化三鐵XRD分析 29
4.1.2 四氧化三鐵對水分散性分析 30
4.1.3 四氧化三鐵磁性分析 31
4.1.4 四氧化三鐵TEM分析 31
4.2 四氧化三鐵與silicalite-1複合材料 34
4.2.1 複合材料實驗結果 34
4.2.2 複合材料XRD分析 34
4.2.3 複合材料TEM、SEM分析 36
4.2.4 複合材料磁特性分析 40
4.2.5 複合材料比表面積比較 41
4.2.6 複合材料外加磁場回收實驗 41
4.3 複合材料血紅蛋白吸附 43
4.3.1 血紅蛋白溶液檢量線製作 43
4.3.2 Langmuir 方程式 44
4.3.3 血紅蛋白的吸附 45
第五章 結論 47
參考文獻 48

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