黏土/聚乙二胺樹枝狀高分子/螢光素鈉之奈米複合材料的製備與研究

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研究生：	李志軒 Chih-hsuan Lee
論文名稱：	黏土/聚乙二胺樹枝狀高分子/螢光素鈉之奈米複合材料的製備與研究 Synthesis and Investigation Of Clay/G4 PAMAM Dendrimer/Uranine Nano-composite material
指導教授：	今榮東洋子 Toyoko Imae
口試委員:	朱義旭 Yi-Hsu Ju 林析右 Shi-Yow Lin 蔡協致 Hsieh-chih Tsai 氏原真樹 Masaki Ujihara
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：	2012
畢業學年度：	100
語文別：	中文
論文頁數：	74
中文關鍵詞：	黏土、樹枝狀高分子、染劑
外文關鍵詞：	Laponite XLG, Dendrimer, Uranine
相關次數：	點閱：165 下載：3
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本研究主要在於探討有機/無機nanocomposite材料之製備與性能。無機材料所使用是黏土(Laponite XLG)，分散於水中，形成脫層型的或插層型的黏土，並添加高分子球(G4 PAMAM Dendrimer)做為連接物，將有機染劑(Uranine)插入，製備成層狀的奈米複合材料的薄膜，並探討其價值及應用性。利用以TEM、UV、FL互相搭配證實插層結構，使Uranine能夠插入複合材料之，並用FL spectra 討論新材料的螢光特性。並將新材料應用在氣體感測上。

使用TEM (Transmission electron microscopy) 觀察奈米複合材料之結構性，在不同pH值的情況下，分析Clay and G4 PAMAM Dendrimer複材有無multilayer的結構，並觀察G4 PAMAM Dendrimer插層在黏土層與層之間的距離與形狀，Clay and G4 PAMAM Dendrimer形成插層結構。

進一步使用FL與UV光譜來分析黏土、染劑與G4 PAMAM Dendrimer各種不同組成的複材，所形成的結構與光學特性。探討染劑有無Quenching現象。以及製備成薄膜後螢光的敏感性。本研究發現所製備出來的奈米複合材料的薄膜，當複材吸附NH3氣體，螢光強度，可作為NH3氣體的探測。

This research is concerning about preparation methods and functions of organic / inorganic nano-composites. The inorganic material is clay (Laponite XLG), which has a layered structure. This clay was dispersed in water to form clear dispersion. To this dispersion, a polymer (G4 polyamideamine dendrimer) was added to hybridize it with the clay. Then, it was confirmed that the precipitated material had a multilayered structure.
To functionalize the clay-dendrimer nano-composite obtained by this method, hybridization of a 3rd component was examined. An organic fluorescent compound, Uranine, was first mixed with the dendrimer solution. Then, hybridization with the clay was performed, typically at pH 8. The obtained material was characterized by transmission electron microscopy and fluorescence spectroscopy.
The nano-composite was confirmed to be multilayer, and its fluorescence was decreased by the hybridization with the dendrimer and mostly quenched at dry condition. Because the fluorescence property of this material varies under different conditions, this material could be applicable for sensing devices.

目錄
摘要................................................................I
Abstract...........................................................II
誌謝..............................................................III
目錄...............................................................IV
表目錄.............................................................VI
圖目錄............................................................VII
第一章	緒論
1-1前言........................................................1
1-2研究動機與目的..............................................2
1-3研究架構....................................................3
第二章	文獻回顧
2-1黏土的性質、Dendrimer與染劑的簡介............................4
		2-1-1人工合成黏土Laponite XLG的簡介........................4
		2-1-2 G4 PAMAM Dendrimer的簡介...............................8
		2-1-3 Uranine的簡介.........................................9
	2-2高分子-黏土奈米複合材料之結構簡介..........................10
	2-3高分子-黏土奈米複合材料之製備簡介..........................13
	2-4高分子-黏土奈米複合材料之性質..............................13
2-5高分子-黏土複合材料的插層結構..............................14
2-6染劑-高分子-黏土複合材料的結構.............................15
第三章	實驗方法與步驟
3-1實驗藥品...................................................20
3-2實驗設備及分析儀器.........................................20
3-3實驗方法...................................................21
		3-3-1 Na+-LAP溶液pKa值分析.................................21
		3-3-2 Na+-LAP溶液製備......................................21
		3-3-3 Na+-LAP/Dendrimer multilayer製備......................21
		3-3-4 Uranine/Dendrimer/Na+-LAP水溶液的製備................22
		3-3-5 Uranine/Dendrimer/Na+-LAP薄膜的製備..................22
	3-4儀器測試與分析.............................................25
第四章	結果與討論
	4-1 Na+-LAP的物理性質與研究....................................26
		4-1-1 觀察黏土行為.........................................26
		4-1-2 Na+-LAP的結構分析....................................27
		4-1-3觀察Na+-LAP加入HCl行為...............................28
		4-1-4 Na+-LAP加入HCl的結構分析.............................29
		4-1-5 Na+-LAP的pKa分析.....................................30
	4-2 Dendrimer/Na+-LAP複合材料的性質與研究......................31
		4-2-1 Na+-LAP與G4 PAMAM Dendrimer的結構分析.................31
		4-2-2 Na+-LAP與G4 PAMAM dendrimer加入HCl的結構分析.........33
		4-2-3 Na+-LAP與G4 PAMAM Dendrimer在不同pH值的結構分析......36
	4-3 Na+-LAP/Dendrimer/Uranine 複合材料的性質與研究..............39
		4-3-1 Uranine的物理性質分析................................39
		4-3-2 Uranine/Na+-LAP複材的物理性質分析....................41
		4-3-3 Uranine/Dendrimer複材的物理性質分析..................43
		4-3-4 Uranine/Dendrimer/Na+-LAP複材的物理性質分析..........45
	4-4 Uranine/Dendrimer/Na+-LAP複材的薄膜應用....................53
4-4-1 Uranine/Dendrimer/Na+-LAP複材薄膜吸收NH3氣體的分析...53
第五章	結論........................................................57
參考文獻...........................................................58
表目錄
表2-1-1不同類型Laponite的性質及應用................................7

















圖目錄
圖2-1 Laponite製備流程圖............................................5
圖2-2 Laponite結構示意圖............................................5
圖2-3 Laponite模板示意圖............................................6
圖2-4 Laponite膨脹示意圖............................................6
圖2-5 G4 PAMAM dendrimer 結構圖......................................8
圖2-6 Uranine在不同pKa下的結構示意圖...............................9
圖2-7相分離型複材示意圖...........................................11
圖2-8插層型奈米複材示意圖.........................................11
圖2-9剝離型奈米複材示意圖.........................................11
圖2-10 Hydrotalicate與G4.5 PAMAM Dendrimer/Hydrotalicate TEM圖......12
圖2-11 G4.5 PAMAM Dendrimer 插入黏土層間而改變形狀示意圖............12
圖2-12染劑aggregation的結果圖.....................................16
圖2-13染劑segregation的結果圖.....................................16
圖2-14染劑integration with clustering的結果圖......................17
圖2-15劑integration的結果圖.......................................17
圖2-16 DEC在不同電荷下的RCMs溶液UV光譜(a)靜置1 min (b)靜置24 hr(虛線為純水溶液無RCMs)...............................................18
圖2-17 boron-dipyrromethene derivative(KBH-01)在不同pH值的(a)UV 與(b)FL光譜圖.......................................................19
圖3-1 Na+-LAP/Dendrimer multilayer製備流程圖........................23
圖3-2 Uranine/Dendrimer/Na+-LAP複材薄膜的氣體探測器製備流程圖......24
圖4-1 Na+-LAP水溶液  實照..........................................26
圖4-2 Na+-LAPG形成膠體的結構.......................................26
圖4-3 Na+-LAP 2wt% 水溶液 TEM 圖....................................27
圖4-4 Na+-LAP加入HCl 實照..........................................28
圖4-5 Na+-LAP加入HCl TEM圖.........................................29
圖4-6 Na+-LAP用HCl 滴定曲線圖......................................30
圖4-7 Na+-LAP與Dendrimer的水溶液 TEM圖............................32
圖4-8 Na+-LAP與Dendrimer加入HCl 的水溶液 TEM圖....................34
圖4-9 Na+-LAP:Dendrimer:HCl 10:10:1的水溶液TEM圖...................35
圖4-10 Laponite XLG和Dendrimer在pH 10的水溶液TEM圖................37
圖4-11 Laponite XLG和Dendrimer 在pH 9的水溶液TEM圖................37
圖4-12 Laponite XLG和Dendrimer 在pH 8的水溶液TEM圖................38
圖4-13 Laponite XLG和Dendrimer插層示意圖...........................38
圖4-14 Uranine 在pH 8的水溶液UV光譜圖.............................39
圖4-15 Uranine 在pH 8的水溶液FL光譜圖.............................40
圖4-16 Uranine/Na+-LAP在pH 8的水溶液UV光譜圖......................41
圖4-17 Uranine/Na+-LAP在pH 8的水溶液FL光譜圖......................42
圖4-18 Uranine/Dendrimer在pH 8水溶液中之UV光譜圖..................44
圖4-19 Uranine/Dendrimer在pH 8水溶液中之FL光譜圖..................44
圖4-20水溶液中Uranine 與Na+-LAP的關係示意圖.......................46
圖4-21 Uranine/Dendrimer/Na+-LAP 在pH 8水溶液中之UV光譜圖..........46
圖4-22 Uranine/Dendrimer/Na+-LAP 在pH 8水溶液中之FL光譜圖..........47
圖4-23 Uranine、Uranine/Na+-LAP、Uranine/Dendrimer、Uranine/ Dendrimer/ Na+-LAP最大螢光強度的波長位置分析圖................................47
圖4-24 Uranine、Uranine/Na+-LAP、Uranine/Dendrimer、Uranine/ Dendrimer /Na+-LAP最大螢光強度分析圖.........................................48
圖4-25 Uranine、Uranine/Na+-LAP、Uranine/Dendrimer、Uranine/ Dendrimer/ Na+-LAP最大UV強度的波長位置分析圖.................................48
圖4-26 Uranine、Uranine/Na+-LAP、Uranine/Dendrimer、Uranine/ Dendrimer/ Na+-LAP最大UV強度分析圖...........................................49
圖4-27利用UV和FL的結果推測Uranine分子在溶液中圖形................51
圖4-28利用UV和FL的結果推測Uranine和Na+-LAP分子在溶液中圖形.......51
圖4-29利用UV和FL的結果推測Uranine和Dendrimer分子在溶液中圖形....52
圖4-30利用UV和FL的結果推測Uranine、Na+-LAP和Dendrimer分子在溶液中圖形...............................................................52
圖4-32 Uranine/Dendrimer/Na+-LAP複材薄膜之最強FL光譜強度...........53
圖4-32為Uranine/Dendrimer/Na+-LAP複材薄膜FL光譜圖強度圖分析.......54
圖4-33 Uranine/Dendrimer/Na+-LAP複材薄膜吸收不同濃度NH3溶液 FL光譜圖.................................................................54
圖4-34 Uranine/Dendrimer/Na+-LAP複材薄膜吸收不同濃度NH3氣體 FL光譜圖強度...............................................................55
圖4-35 Uranine/Dendrimer/Na+-LAP與NH3的互相反應示意圖..............56

                                

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