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微/介孔複合孔洞材料之合成、鑑定與應用之研究 = The study o...
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國立高雄大學應用化學系碩士班
微/介孔複合孔洞材料之合成、鑑定與應用之研究 = The study of the hierarchical material's synthesis, analysis and application
紀錄類型:
書目-語言資料,印刷品 : 單行本
並列題名:
The study of the hierarchical material's synthesis, analysis and application
作者:
趙倍賢,
其他團體作者:
國立高雄大學
出版地:
[高雄市]
出版者:
撰者;
出版年:
2008[民97]
面頁冊數:
103面圖,表 : 30公分;
標題:
微/介孔複合孔洞材料
標題:
hierarchical material
電子資源:
http://handle.ncl.edu.tw/11296/ndltd/56748212789141428721
附註:
指導教授:蔡振章
附註:
參考書目:面86-90
摘要註:
製備微/介孔複合孔洞材料兼具沸石結晶構造與介孔孔洞結構,可結合微孔沸石與介孔分子篩之優點,提高分子擴散係數。本研究探討微/介孔複合孔洞材料之製備方法、孔洞結構鑑定,與催化應用。 在材料製備方面,吾人成功合成超高水熱穩定性MCM-41,經過760℃水蒸氣處理超過一天,依然維持良好之孔洞結構,該超穩結構不是因為壁厚增加所造成,可能來自於改良之合成條件。此外,利用離子拓印後處理MCM-41能夠提高熱穩定性。另一方面,以沸石材料為原料,利用後再結晶法與鹼溶解法,製備微介孔複合孔洞材料。 MFI沸石經由鹼處理法形成微/介孔複合孔洞結構,分段式鹼處理效果較佳,全段式鹼處理容易導致SiO2回填,降低十圓環孔洞口徑。於正己烷異構化反應,該複合孔洞沸石提高約50C催化活性,突破微孔對於DMB產率之產物分子尺度限制,開拓新型催化途徑之可能性。同時,以大分子有機鹼quinoline進行選擇性毒化實驗,推論該複合孔洞為微孔與介孔孔道交聯結構。相對的,後再結晶合成法製得複合孔洞材料屬於非交聯孔道結構,其催化性能與MFI沸石相同。另外亦發現微/介孔複合型mordenite沸石在重芳香烴轉烷化反應之催化穩定性明顯改善,效果相當於Pt/mordenite催化穩定性。 Hierarchical material combining microporous and mesoporous structure possesses the merits of microporous zeolite and mesoporous material. The hierarchical porous structure could enhance molecular diffusivity and also catalytic properties. This research aims at the preparation and characterization as well as catalytic application of hierarchical material. On the material preparation aspect, we have successfully prepared a super hydrothermal stable MCM-41 which is tolerant for steaming treatment at 760C for more than 24 hours. The stability is attributed to the improved synthesis conditions at low basicity, rather than from higher wall thickness. Furthermore, the thermal stability of MCM-41 can be improved by ion-imprinting treatment. On the other hand, hierarchical material can be prepared from zeolite samples by re-crystallization and base leaching treatment. It was found that in the preparation of hierarchical material, multiple treatment procedure is more effective. Single treatment procedure with extending treating time tends to plug the micropores of zeolite by the dissolved silica. In the hexane isomerization over MFI, dimethylbutane (DMB) yield is limited by the 10-membered oxygen ring pore. The hierarchical porous structure in MFI zeolite can enhance catalytic activity by about 50C and produce high DMB yield. The finding explores a new direction to extending the application of zeolite outside the limitation of pore diameters. In addition, based on the temperature programming desorption of hexane isomers and selective poisoning of quinoline, it is proposed that the microporores and mesopores of hierarchical MFI are interconnected. In contrast, the catalytic activity of hierarchical MFI prepared by re-crystallization is similar with that of regular MFI zeolite. Furthermore, the micropore and mesopore are not interconnected. It was also found that the hierarchical mordenite can improve significantly the catalytic stability of mordenite comparable to Pt/mordenite in heavy aromatics transalkylation.
微/介孔複合孔洞材料之合成、鑑定與應用之研究 = The study of the hierarchical material's synthesis, analysis and application
趙, 倍賢
微/介孔複合孔洞材料之合成、鑑定與應用之研究
= The study of the hierarchical material's synthesis, analysis and application / 趙倍賢撰 - [高雄市] : 撰者, 2008[民97]. - 103面 ; 圖,表 ; 30公分.
指導教授:蔡振章參考書目:面86-90.
微/介孔複合孔洞材料hierarchical material
微/介孔複合孔洞材料之合成、鑑定與應用之研究 = The study of the hierarchical material's synthesis, analysis and application
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製備微/介孔複合孔洞材料兼具沸石結晶構造與介孔孔洞結構,可結合微孔沸石與介孔分子篩之優點,提高分子擴散係數。本研究探討微/介孔複合孔洞材料之製備方法、孔洞結構鑑定,與催化應用。 在材料製備方面,吾人成功合成超高水熱穩定性MCM-41,經過760℃水蒸氣處理超過一天,依然維持良好之孔洞結構,該超穩結構不是因為壁厚增加所造成,可能來自於改良之合成條件。此外,利用離子拓印後處理MCM-41能夠提高熱穩定性。另一方面,以沸石材料為原料,利用後再結晶法與鹼溶解法,製備微介孔複合孔洞材料。 MFI沸石經由鹼處理法形成微/介孔複合孔洞結構,分段式鹼處理效果較佳,全段式鹼處理容易導致SiO2回填,降低十圓環孔洞口徑。於正己烷異構化反應,該複合孔洞沸石提高約50C催化活性,突破微孔對於DMB產率之產物分子尺度限制,開拓新型催化途徑之可能性。同時,以大分子有機鹼quinoline進行選擇性毒化實驗,推論該複合孔洞為微孔與介孔孔道交聯結構。相對的,後再結晶合成法製得複合孔洞材料屬於非交聯孔道結構,其催化性能與MFI沸石相同。另外亦發現微/介孔複合型mordenite沸石在重芳香烴轉烷化反應之催化穩定性明顯改善,效果相當於Pt/mordenite催化穩定性。 Hierarchical material combining microporous and mesoporous structure possesses the merits of microporous zeolite and mesoporous material. The hierarchical porous structure could enhance molecular diffusivity and also catalytic properties. This research aims at the preparation and characterization as well as catalytic application of hierarchical material. On the material preparation aspect, we have successfully prepared a super hydrothermal stable MCM-41 which is tolerant for steaming treatment at 760C for more than 24 hours. The stability is attributed to the improved synthesis conditions at low basicity, rather than from higher wall thickness. Furthermore, the thermal stability of MCM-41 can be improved by ion-imprinting treatment. On the other hand, hierarchical material can be prepared from zeolite samples by re-crystallization and base leaching treatment. It was found that in the preparation of hierarchical material, multiple treatment procedure is more effective. Single treatment procedure with extending treating time tends to plug the micropores of zeolite by the dissolved silica. In the hexane isomerization over MFI, dimethylbutane (DMB) yield is limited by the 10-membered oxygen ring pore. The hierarchical porous structure in MFI zeolite can enhance catalytic activity by about 50C and produce high DMB yield. The finding explores a new direction to extending the application of zeolite outside the limitation of pore diameters. In addition, based on the temperature programming desorption of hexane isomers and selective poisoning of quinoline, it is proposed that the microporores and mesopores of hierarchical MFI are interconnected. In contrast, the catalytic activity of hierarchical MFI prepared by re-crystallization is similar with that of regular MFI zeolite. Furthermore, the micropore and mesopore are not interconnected. It was also found that the hierarchical mordenite can improve significantly the catalytic stability of mordenite comparable to Pt/mordenite in heavy aromatics transalkylation.
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http://handle.ncl.edu.tw/11296/ndltd/56748212789141428721
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