MFI奈米沸石粒子的形貌控制

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姓名

許群侑(Chun-Yu Hsu) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

MFI奈米沸石粒子的形貌控制
(Morphology control of MFI zeolite)

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摘要(中)

實驗室過去已經發展出一套奈米silicalite-1的合成方法，可快速製作出尺寸50~60 nm粒子、且均一分佈的奈米沸石。
本研究是以過去的方法為基礎並改變不同反應條件，製作出兩種不同形貌的沸石且尺寸與過去相近。為了探討不同結構的反應機制，將不同條件下製作出的產物進行分析。主要分析部份為離心上下層產率、表面形態(SEM、TEM)、表面官能基(FTIR)、結晶性及晶體結構(XRD)、比表面積孔徑分佈(ASAP)、粒徑分佈(DLS)等。
鍛燒後，兩種不同形貌沸石的再分散性也有明顯差異。在鹼性溶液下，單晶粒子較複合結晶粒子有分散性(PDI<0.1)。並且粒子經過MPS表面改質可分散至MEK，未來將有機會混入高分子，製作出低折率材料。
利用稀釋前驅濃膠到不同醇類中，合成出不同形貌的粒子。另外，改變不同低溫反應時間，也可得到不同尺寸的沸石粒子。

摘要(英)

A rapid synthesis procedure for silicalite-1 nanocrystals was developed in our laboratory in the past. The crystal sizes about 50 nm are uniform.
In the study, the previous synthesis procedure were modified to produce silicalite-1 nanocrystals with similar size but different morphologies. To study the growth mechanisms of nanocrystals in different morphologies, the products were analyzed with FTIR, SEM, TEM, ASAP and centrifuged yield .
After calcination, the dispersion is different for well-shaped and agglomerated nanocrystals. The well-shaped nanocrystals were dispersed much better in alkaline solution after calcination than agglomerated nanocrystals and the dispersed particles were uniform(PDI<0.1). The well-shaped nanocrystals dispersed in MEK by surface modification with MPS. It might be applied in hybrid materials.
The particles in different morphologies can be synthesized by diluting precussor in alcohols. In addition, the different size particles were obtained by different aging time.

關鍵字(中)

★ MFI奈米沸石粒子的形貌控制

關鍵字(英)

★ Morpholoy control of MFI zeolite

論文目次

目錄
摘要 I
Abstract II
誌謝 III
目錄 IV
圖目錄 VI
表目錄 IX
第一章序論 1
1-1 沸石簡介 1
1-2 MFI沸石 2
第二章文獻回顧 3
2-1 沸石前驅液的研究 3
2-2 奈米級MFI沸石合成 5
2-3 微米級沸石合成 5
2-4 利用不同合成方式控制沸石形貌 6
2-5 研究方向 7
第三章沸石前驅物製備與儀器樣品製備方法 8
3-1 實驗藥品 8
3-2 沸石前驅物及兩段式加熱合成奈米MFI沸石 9
3-2-1 備置澄清溶液 9
3-2-2 離心清洗 12
3-2-3 利用醇類將粒子表面進行改質 13
3-2-4 高溫鍛燒及重新獲得分散奈米沸石 14
3-3 高水比下備置次微米粒子及微米沸石 14
3-3-1 透明前驅液製備方式 14
3-3-2 離心清洗與製備親水矽晶片 15
3-3-3 利用塗抹方式將乾燥粉體塗抹成單層排列 15
3-4 Silicalite-1的鑑定與分析 16
3-4-1 動態雷射粒徑儀(DLS)分析 16
3-4-2 傅立葉紅外線光譜儀(FTIR)分析 16
3-4-3 粉末式X光繞射(PXRD)分析 17
3-4-4 掃描式電子顯微鏡(SEM) 17
3-4-5 熱重損失(TGA)分析 17
3-4-6 穿透式電子顯微鏡(TEM)分析 17
3-4-7 氮氣恆溫吸附(ASAP)分析 18
第四章結果與討論 19
4-1 利用濃縮老化及二段式加熱製備奈米沸石 19
4-2 沸石聚集結晶機制 20
4-2-1 不同老化時間對粒子形貌的影響 22
4-2-2 不同形貌對氮氣吸附的影響 26
4-2-3 離心上下層的分析與鑑定 29
4-2-3-1 離心上下層的分析(FTIR及XRD) 29
4-2-3-2 老化時間對結晶量的影響 33
4-2-4 影響沸石形貌的成長機制 35
4-3 有機相合成沸石 37
4-3-1 有機溶劑對沸石聚集影響 37
4-3-2 老化時間對粒子大小之差異性 38
4-3-3 沸石鑑定與分析(FTIR、XRD) 41
4-4 利用不同醇類進行表面改質 43
4-5 鍛燒後沸石的再分散性 44
4-6 高水比下合成微米沸石 47
4-6-1 有無濃縮對粒子大小差異(SEM) 47
4-6-2 利用微米級沸石製備b軸朝上沸石膜(XRD) 48
第五章結論與建議 50

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指導教授

蔣孝澈(A.S.T. Chiang)

審核日期

2010-7-26

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