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研究生:陳寶森
研究生(外文):Pao-Sen Chen
論文名稱:奈米沸石TS-1之合成及其特性分析
論文名稱(外文):A Facile Method For The Synthesis of Nanocrystalline Zeolite TS-1
指導教授:許秀菱許秀菱引用關係
指導教授(外文):Hsiu-Ling Hsu
學位類別:碩士
校院名稱:龍華科技大學
系所名稱:工程技術研究所
學門:工程學門
學類:綜合工程學類
論文種類:學術論文
論文出版年:2007
畢業學年度:95
語文別:中文
論文頁數:86
中文關鍵詞:溶膠-凝膠法真空減壓濃縮法水熱法TS-1
外文關鍵詞:sol-gelConcentration methodHydrothermal methodTS-1
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本研究主要是藉由改變藥品TBOT克數及熟化時間,並利用溶膠-凝膠法製備TS-1沸石之前驅物,再經由改良文獻製程後增加之步驟:『真空減壓濃縮法』改變前驅溶膠之成分比例,並移去水解後產生之醇類與樣品所含之水分,即可得到一高濃度的TS-1沸石前驅物之透明溶膠,再將此溶膠以80oC溫度加熱以增加晶核濃度,加熱一段時間之後,再將此前驅物溶膠以175oC水熱法反應,使前驅物溶膠晶核轉化為奈米結晶。將此溶膠取樣均勻分散於水中,並以雷射粒徑分析儀(DLS)來分析沸石結晶之粒子粒徑大小以及粒子之分散情形,確定為分散之奈米分散液,再將此含奈米結晶之溶膠乾燥,得到一透明固態之結晶溶膠,研磨成粉狀後,以紅外光譜(FT-IR)、X光射線繞射儀(XRD)、掃描式電子顯微鏡(SEM)以及穿隧式電子顯微鏡(TEM)等儀器做檢測,而由以上這些儀器檢測可知,利用本研究所改良之方法及步驟可以成功的製備出粒子大小介於70 nm至80 nm之TS-1沸石,並且可以將合成之時間從文獻值的190天縮短為2天。
This research is mainly to get a translucent solid : Nano Zeolite TS-1. It is prepared by sol-gel method , concentration method and hydrothermal method . Following methods are adopted in the synthesis of nano zeoliteTS-1 . In sol-gel method , the precursor is prepared by varying the molar concentration of TBOT . The solution is concentrated at 80oC, resulting in the formation of gel . The resultant gel transferred into stainless steel autoclave and subjected to hydrothermal reaction at 175oC for 90 min . The resultant nano crystals were characterized by Dynamic light scattering (DLS) , Fourier Transform Infrared Spectroscopy (FT-IR) , X-ray diffraction (XRD) , Field-Emission Scanning Electron Microscope (FE-SEM) and Transmission Electron Microscope (TEM) . This result shows that, with this procedure we can prepare the TS-1 in 2 days with the particle size between 70~80 nm where as in the literature TS-1 is prepared in 190 days.
目錄

第一章 緒論.........................................................................................................1
1.1 研究動機..................................................................................................1
1.2 研究目的..................................................................................................1
1.3 沸石介紹..................................................................................................2
1.4 MFI沸石之形成.......................................................................................4
1.5 MFI-ZSM-5型沸石介紹...........................................................................6
1.6 奈米級沸石的應用...................................................................................7
1.7 鈦矽沸石之探討.......................................................................................8
第二章 實驗原理……………...............................................................................11
2.1實驗原理……………….............................................................................11
2.2實驗方法….............................................................................11
2.2.1溶膠-凝膠法…............................................................................11
2.2.2真空減壓濃縮法...............................................................................13
2.2.3水熱法................................................................................13
2.3使用之儀器介紹….............................................................................14
2.3.1 XRD介紹…..........................................................................14
2.3.2 SEM 介紹....................................................................................15
2.3.3 TEM介紹......................................................................................16
2.3.4 DLS介紹................................................................................17
2.3.5 FT-IR介紹................................................................................18
第三章 實驗步驟..................................................................................................20
3.1實驗藥品....................................................................................................20
3.2實驗儀器....................................................................................................21
3.3實驗步驟..................................................................................................22
3.3.1利用濃縮及水熱法合成奈米級TS-1觸媒........................................22
3.3.2 TS-1沸石前驅物之配製…...............................................................23
3.3.3 TS-1沸石之合成.............................................................................23
3.4實驗檢測與分析......................................................................................28
第四章 結果與討論............................................................................................29
4.1雷射粒徑分析儀分析…...........................................................................30
4.2場效式電子顯微鏡分析...........................................................................32
4.3穿隧式電子顯微鏡分析...........................................................................41
4.4 X射線繞射分析..........................................................................45
4.5紅外線光譜分析...........................................................................47
第五章 結論….....................................................................................................53
參考文獻………....................................................................................................54
附表:實驗之步驟紀錄及各檢測圖表…..............................................................59











圖目錄

圖1-1 ZSM-5沸石結構 .......................................................................................6
圖2-1 本研究使用之XRD機台照片(LHU) .......................................................15
圖2-2 本研究使用之SEM機台照片(LHU) .......................................................16
圖2-3 研究使用之TEM機台照片(台大農業昆蟲系) ........................................17
圖2-4 本研究使用之DLS機台照片(LHU) ........................................................18
圖2-5 本研究使用之FT-IR機台照片(LHU) ....................................................19
圖3-1 本研究使用之旋轉濃縮機照片(LHU) .....................................................21
圖3-2 本研究使用之精密烘箱照片(LHU) .........................................................21
圖3-3 本研究使用之精密電子天秤照片(LHU) .................................................22
圖3-4 本研究使用之pH計照片(LHU) ..............................................................22
圖3-5 本研究之實驗流程圖 ..............................................................................27
圖4-1 Sample 2-10之DLS分析圖....................................................................30
圖4-2 Sample 2 (TBOT=1g,ageing time=1.5days,NC-36)之SEM照片 ......32
圖4-3 Sample 3 (TBOT=1g,ageing time=1.5days,NC-36)之SEM照片 ......32
圖4-4 Sample 4 (TBOT=1g,ageing time=1.5days,NC-36)之SEM照片 ......33
圖4-5 Sample 5 (TBOT=2g,ageing time=1.5days,NC-36)之SEM照片 ......33
圖4-6 Sample 6 (TBOT=2g,ageing time=1.5days,NC-36)之SEM照片 ........34圖4-7 Sample 11 (TBOT=1g,ageing time=1.5days,NC-36)之SEM照片 ......34圖4-8 Sample 12 (TBOT=1g,ageing time=5days,CP-36)之SEM照片 .........35圖4-9 Sample 13 (TBOT=2g,ageing time=8days,CP-36)之SEM照片 .........35圖4-10 Sample 14 (TBOT=1g,ageing time=1.5days,CP-36)之SEM照片 .......36
圖4-11 Sample 15 (TBOT=2g,ageing time=10days,CP-36)之SEM照片 ........36
圖4-12 Sample 16 (TBOT=2g,ageing time=5days,CP-36)之SEM照片 ........37圖 4-13 Sample 17 (TBOT=1g,ageing time=1.5days,NC-36)之SEM照片 .....37圖 4-14 Sample 18 (TBOT=1g,ageing time=1.5days,NC-36) 之SEM照片 ....38圖 4-15 Sample 19 (TBOT=1g,ageing time=7days,CP-36)之SEM照片 ........38
圖 4-16 Sample 20 (TBOT=2g,ageing time=1.5days,CP-36)之SEM照片 .....39
圖 4-17 Sample 2 (TBOT=1g,ageing time=1.5days,NC-36)之TEM照片 .....41圖 4-18 Sample 3 (TBOT=1g,ageing time=1.5days,NC-36)之TEM照片 .....41
圖 4-19 Sample 4 (TBOT=1g,ageing time=1.5days,NC-36)之TEM照片 .....42圖 4-20 Sample 11 (TBOT=1g,ageing time=1.5days,NC-36)之TEM照片 .....42圖 4-21 Sample 12 (TBOT=1g,ageing time=5days,CP-36)之TEM照片 ........43圖 4-22 Sample 13 (TBOT=2g,ageing time=8days,CP-36)之TEM照片 ........43
圖 4-23 Sample 14 (TBOT=1g,ageing time=1.5days,CP-36)之TEM照片 .....44圖 4-24各sample之XRD分析圖 .........................................................................45
圖 4-25 Sample 11 (TBOT=1g,ageing time=1.5days,NC-36)之FT-IR分析圖 .47
圖 4-25 Sample 12 (TBOT=1g,ageing time=5days,CP-36)之FT-IR分析圖 ....47
圖 4-27 Sample 13 (TBOT=2g,ageing time=8days,CP-36)之FT-IR分析圖 ....48
圖 4-28 Sample 14 (TBOT=1g,ageing time=1.5days,CP-36)之FT-IR分析圖 .48
圖 4-29 Sample 15 (TBOT=2g,ageing time=10days,CP-36)之FT-IR分析圖 ..49
圖 4-30 Sample 16 (TBOT=2g,ageing time=5days,CP-36)之FT-IR分析圖 ....49
圖 4-31 Sample 17 (TBOT=1g,ageing time=1.5days,NC-36)之FT-IR分析圖 .50
圖 4-32 Sample 18 (TBOT=1g,ageing time=1.5days,NC-36)之FT-IR分析圖 .50
圖 4-33 Sample 19 (TBOT=1g,ageing time=7days,CP-36)之FT-IR分析圖 ....51
圖 4-34 Sample 20 (TBOT=2g,ageing time=1.5days,CP-36)之FT-IR分析圖 .51



表目錄

表1-1業界與研究中常見之沸石種類列表.............................................................4
表1-2奈米級沸石之應用........................................................................................7
表2-1紅外線光譜區.............................................................................................19
表3-1本實驗製備TS-1沸石之各反應物重量及熟化時間條件設計表...............24
表3-2本實驗製備TS-1沸石之各反應物重量、反應方法及熟化時間條件表.....25
表3-3本研究使用之檢測儀器及其參數設定整理表……………........................28
表4-1 Sample檢測一覽表.........................................…………….......................29
表4-2 DLS粒徑整理表..............................................…………….......................31
表4-3 SEM結果整理表.......................................................................................40
表4-4 TEM粒子分散度比較表...........................................................................44
表4-5 各XRD樣品之合成參數.............................................................................46
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