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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 萬本儒(Ben-Zu Wan) | |
| dc.contributor.author | Yi-Hsiu Chen | en |
| dc.contributor.author | 陳怡秀 | zh_TW |
| dc.date.accessioned | 2021-06-15T03:03:34Z | - |
| dc.date.available | 2012-08-03 | |
| dc.date.copyright | 2009-08-03 | |
| dc.date.issued | 2009 | |
| dc.date.submitted | 2009-07-30 | |
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Ichikawa, 'Studies of the selective reduction of nitric oxide by carbon monoxide in the presence and absence of hydrogen over Au/NaY catalysts,' Journal of the Chemical Society-Faraday Transactions, vol. 92, pp. 301-306, Jan 21 1996. [31] S. L. Qiu, R. Ohnishi, and M. Ichikawa, 'Formation and Interaction of Carbonyls and Nitrosyls on Gold(I) in Zsm-5 Zeolite Catalytically Active in No Reduction with Co,' Journal of Physical Chemistry, vol. 98, pp. 2719-2721, Mar 17 1994. [32] E. Smolentseva, A. Pestryakov, N. Bogdanchikova, A. Simakov, M. Avalos, M. Farias, J. Diaz, V. Gurin, and A. Tompos, 'Influence of Fe introduction method on gold state in NaY zeolite,' International Journal of Modern Physics B, vol. 19, pp. 2496-2501, Jul 10 2005. [33] J. C. Fierro-Gonzalez, Y. L. Hao, and B. C. Gates, 'Gold nanoclusters entrapped in the alpha-cages of Y zeolites: Structural characterization by X-ray absorption spectroscopy,' Journal of Physical Chemistry C, vol. 111, pp. 6645-6651, May 10 2007. 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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/44535 | - |
| dc.description.abstract | 本研究以氯化金酸為前軀物，Y型沸石為擔體，在溶液中將金載負於擔體上製備Au/Y觸媒，在0℃溫度下催化一氧化碳氧化反應，鑑定工具為AA、TPR、HRTEM、SEM、solid-state NMR、XRD和TGA。研究主要分為三部分。首先，嘗試就以下製程變因：(1) 修飾擔體溶液的pH值，(2) 擔體乾燥方式，了解製程變化對觸媒活性的影響，並探討金載負於擔體的機制。第二，為了解觸媒催化反應過程中，累積的熱量（一氧化碳氧化反應為放熱反應）對觸媒活性造成的影響，設計以下兩種變因：(1) 透過觸媒製備中的擔體用量控制Au/Y的金載負量，以及(2)反應中用以幫助熱傳的石英砂用量，探討熱傳效應在觸媒催化反應中所扮演的角色。第三，在相同程序下所製備的Au/Y中，會有明顯的金載負量差異，研究結果顯示製備觸媒的pH值微量變化會對金載負量有顯著的影響，因此本研究結論出一製備程序，透過有效地控制製程中金溶液pH值，解決相同製程下金載負量差異的問題。
以下是部份的研究成果：(1) 相較於室溫和60℃乾燥的沸石，金於未經乾燥之沸石載負量最低， (2) 修飾沸石的溶液pH值越低，則金的載負量越高， (3) 由XRD和SEM的鑑定結果指出，沸石的修飾過程對晶體結構會產生破壞，然而，金在沒有經過任何修飾過的沸石上載負量卻是最低的， (4) 比較室溫乾燥和60℃乾燥沸石的solid-state NMR鑑定結果，發現室溫乾燥的沸石含有較多的OH基，而金於室溫乾燥下沸石的載負量大於60℃乾燥下的沸石。 本研究針對金載負於Y型沸石的機制，提出以下可能的情況：(1) 當乾燥的Y型沸石放入金溶液時，沸石吸收溶液的程序使金化合物初步的沈積於沸石孔洞內，(2) H＋催化脫水反應形成更多金化合物的鍵結，(3) 沸石結構損壞有助於金化合物擴散及吸附於孔洞內部，(4) 沸石內部OH基與金化合物脫水形成鍵結。 針對石英砂用量對觸媒活性影響，結果顯示，石英砂的添加有助於觸媒活性穩定度的提升，這是因為石英砂可以幫助熱傳以及減少觸媒內部熱的累積。此外，比較金載負量差異對觸媒活性的影響，高載負量的Au/Y雖然有較高的催化活性，但活性穩定性明顯較差。綜合以上結果，由於沸石的孔洞結構，熱傳導能力不佳，一氧化碳氧化反應所釋放的熱能會累積於觸媒內部，熱能不但有助於提升初始反應時金的還原速率(活化金的催化能力)，同時也會提升觸媒內部的溫度而加快氧化反應速率。然而過多的熱量累積也會造成金顆粒的聚集，導致Au/Y觸媒活性的衰退，此一現象在金載負量較高的Au/Y觸媒活性表現中尤其明顯。 | zh_TW |
| dc.description.provenance | Made available in DSpace on 2021-06-15T03:03:34Z (GMT). No. of bitstreams: 1 ntu-98-R96524045-1.pdf: 3404284 bytes, checksum: 3e23ef8ec474b5946f6405dc6f289887 (MD5) Previous issue date: 2009 | en |
| dc.description.tableofcontents | 摘要……………………………… I
Abstract………………………… III 目錄…………………… V 圖索引………………… VIII 表索引……………….. XI 第一章 緒論…………. 1 1-1 研究動機 1 1-2 研究背景 3 1-3 研究方向 4 第二章 文獻回顧 6 2-1 金觸媒的發展 6 2-2 沸石Y的介紹 7 2-3 金觸媒製備方式 10 2-3-1 含浸法 (Impregnation, IMP or Incipient wetness, IW) 10 2-3-2 共沈澱法 (Co-Precipitation) 11 2-3-3 沈澱沈積法 (Deposition Preciptation, DP) 12 2-3-4 離子交換法 (Ion Exchange, IE) 13 2-4 AuY觸媒的發展 14 第三章 實驗與鑑定方法 17 3-1 實驗藥品和器材 17 3-1-1 實驗藥品來源 17 3-1-2 反應氣體來源 18 3-1-3 實驗使用器材 18 3-2 Au/Y 觸媒製備 19 3-2-1 擔體Y表面處理程序 19 3-2-2 Au/Y 觸媒製備程序 20 3-3 觸媒鑑定 22 3-3-1 原子吸收光譜儀 (AA) 22 3-3-2 高解析穿透式電子顯微鏡 (HRTEM) 22 3-3-3 X射線繞射光譜儀 (XRD) 23 3-3-4 熱重分析 (TGA) 23 3-3-5 掃描式電子顯微鏡 (SEM) 24 3-3-6 固態核磁共振 (solid-state NMR) 24 3-3-7 程溫規劃還原 (TPR) 25 3-4 觸媒活性測試 27 第四章 研究結果 29 4-1 修飾擔體之pH值的影響 29 4-1-1 Au/Y的製備與元素分析 (AA) 29 4-1-2 活性測試 30 4-1-3 程溫規劃還原 (TPR) 31 4-1-4 紫外光/可見光光譜 (UV/vis) 31 4-1-5 X-射線繞射光譜 (XRD) 33 4-1-6 穿透式電子顯微鏡 (HRTEM) 33 4-1-6-1 鑑定結果 33 4-1-6-2 反應前後顆粒大小統計 (particle size distribution) 36 4-1-7 掃描式電子顯微鏡 (SEM) 37 4-2 擔體乾燥之影響 39 4-2-1 觸媒的製備與元素分析 (AA) 39 4-2-2 活性測試 40 4-2-3 高磁場核磁共振儀 (solid-state NMR) 40 4-2-4 X-射線繞射光譜 (XRD) 45 4-2-5 熱重分析 (TGA) 46 4-3 擔體添加量對製備Au/Y之影響 47 4-3-1 觸媒的製備與元素分析 (AA) 47 4-3-2 活性測試 47 4-3-3 程溫規劃還原 (TPR) 48 4-3-4 穿透式電子顯微鏡 (HRTEM) 49 4-3-4-1 鑑定結果 49 4-3-4-2 反應前後顆粒大小統計 (particle size distribution) 51 4-4 反應過程添加石英砂之影響 52 4-4-1 觸媒的製備與元素分析 (AA) 52 4-4-2 活性測試 53 4-4-3 穿透式電子顯微鏡 (HRTEM) 54 4-4-3-1 鑑定結果 54 4-4-3-2 反應前後顆粒大小統計 (particle size distribution) 56 第五章 研究討論 57 5-1 Au載負機制 57 5-1-1 金溶液灌入乾燥擔體帶入Au沈積於沸石孔洞內 57 5-1-2 H＋催化金錯合物脫水形成鍵結 58 5-1-3 沸石結構損壞有助於金載負於孔洞內部 61 5-1-4 沸石內部OH基與金錯合物脫水形成鍵結 64 5-1-5 結論 66 5-2 Au/Y觸媒催化一氧化碳氧化反應 66 5-2-1 活性位置 66 5-2-2 熱傳效應 67 5-2-3 顆粒位置影響催化穩定性 73 5-2-4 加入石英砂加速熱傳 77 5-2-5 結論 79 5-3 金載負量再現性探討 80 5-3-1 金載負量再現性問題 80 5-3-2 Au/Y製備流程 81 5-3-3 分析討論 82 5-3-4 製程改善 84 5-3-5 結果討論 86 5-3-6 結論 88 第六章 結論…… 89 第七章 參考文獻 91 | |
| dc.language.iso | zh-TW | |
| dc.title | Au/Y製備及催化一氧化碳氧化反應之熱傳效應探討 | zh_TW |
| dc.title | Study on Au/Y Preparation and Heat Transfer Effects on CO Oxidation | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 97-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 林俊男(Jiunn-Nan Lin),郭錦龍(Chin-Lung Kuo) | |
| dc.subject.keyword | Au/Y觸媒,Y型沸石,一氧化碳氧化反應,熱傳效應, | zh_TW |
| dc.subject.keyword | Au/Y catalyst,Y-type zeolite,CO oxidation,heat transfer effect, | en |
| dc.relation.page | 94 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2009-07-30 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
| 顯示於系所單位： | 化學工程學系 | |
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