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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/79626完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 游文岳(Wen-Yueh Yu) | |
| dc.contributor.author | Po-Wei Chen | en |
| dc.contributor.author | 陳柏瑋 | zh_TW |
| dc.date.accessioned | 2022-11-23T09:05:38Z | - |
| dc.date.available | 2026-09-26 | |
| dc.date.available | 2022-11-23T09:05:38Z | - |
| dc.date.copyright | 2021-11-09 | |
| dc.date.issued | 2021 | |
| dc.date.submitted | 2021-09-30 | |
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The Journal of Physical Chemistry 1986, 90 (14), 3148-3152. [45] M. Waqif, P. Bazin, O. Saur, J. Lavalley, G. Blanchard, and O. Touret, 'Study of ceria sulfation.' Applied Catalysis B: Environmental 1997, 11 (2), 193-205. [46] S. D. Lin, A. C. Gluhoi, and B. E. Nieuwenhuys, 'Ammonia oxidation over Au/MOx/γ-Al2O3 — activity, selectivity and FTIR measurements.' Catalysis today 2004, 90 (1-2), 3-14. [47] L. Liu, B. Liu, L. Dong, J. Zhu, H. Wan, K. Sun, B. Zhao, H. Zhu, L. Dong, and Y. Chen, 'In situ FT-infrared investigation of CO or/and NO interaction with CuO/Ce0.67Zr0.33O2 catalysts.' Applied Catalysis B: Environmental 2009, 90 (3-4), 578-586. [48] L. Zhang, J. Pierce, V. L. Leung, D. Wang, and W. S. Epling, 'Characterization of ceria’s interaction with NOx and NH3.' The Journal of Physical Chemistry C 2013, 117 (16), 8282-8289. [49] B. Azambre, L. Zenboury, A. Koch, and J. 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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/79626 | - |
| dc.description.abstract | "工廠與汽車所排放的氮氧化物(Nitrogen oxide, NOx)造成非常嚴重的環境汙染，如酸雨、光化學霧霾以及PM2.5，選擇性觸媒還原(selectivity catalytic reduction, SCR)反應通常被應用在脫除氮氧化物，V2O5-WO3/TiO2商業觸媒長久以來已經被廣泛的應用在SCR反應，然而五氧化二釩被世界衛生組織視為人類潛在的致癌物質，而被分類為group 2B，因此尋找可以替代V2O5-WO3/TiO2觸媒已成為一項急迫的工作。文獻報導指出CeO2由於具有強還原性質與氧儲存能力，因此成為具潛力的替代觸媒，最近研究指出在以在無氧條件(anaerobic)下以SO2硫化處理CeO2可以大幅提升反應活性。 本研究中，我們在無氧條件下以500 ppm SO2/Ar氣體硫化處理CeO2觸媒，改變硫化處理溫度與時間的變因: 在200、300、400與500 oC硫化處理30分鐘，以及在300 oC硫化處理5、15、30與120分鐘，並測試硫化處理後CeO2觸媒於選擇性脫硝還原(SCR)反應的活性，分析硫化處理溫度與時間的變因對硫化物在觸媒表面上形成的影響。我們發現硫化處理溫度200 – 500 oC改善觸媒活性的效果相同；在不同硫化處理時間下，以硫化處理30分鐘，觸媒活性即達到最佳表現，可能原因為CeO2表面的chelating sulfate達到飽和。CeO2主要為路易士酸性位點，而硫化處理後CeO2則為路易士與布羅忍斯特酸性位點，布羅忍斯特酸性位點使NH3吸附量大幅提升。在NH3升溫IR實驗中，我們確認表面sulfate為布羅忍斯特酸性位點，而sulfate並不影響原有的路易士酸性位點存在。CeO2上的NH3容易進行H-abstraction而形成N2O與NO等副產物，而硫化處理後CeO2則抑制NH3進行H-abstraction。由於NO吸附位點被sulfate占據，因此硫化處理後CeO2的NO吸附量大幅下降。在in-situ IR實驗中，我們可以得知CeO2上imide species容易與氣相NO反應，而nitrate卻不易與氣相NH3反應；硫化處理後的CeO2上之NH3與NH4+容易與氣相NO進行反應，然而硫化處理後的CeO2的NO吸附量較少，因此我們推測兩者主要皆以Eley-Rideal機制進行反應。 " | zh_TW |
| dc.description.provenance | Made available in DSpace on 2022-11-23T09:05:38Z (GMT). No. of bitstreams: 1 U0001-0809202115562900.pdf: 4670343 bytes, checksum: 184f1d0ce63f6d1d96903270e3ae7307 (MD5) Previous issue date: 2021 | en |
| dc.description.tableofcontents | 口試委員會審定書 i 致謝 ii 摘要 iv Abstract v 目錄 vi 圖目錄 ix 表目錄 xii 第一章 緒論 1 1.1 研究背景 1 1.1.1 氮氧化物對環境汙染之影響 1 1.1.2 脫除氮氧化物之技術 1 1.2 反應介紹 3 1.2.1 選擇性觸媒還原反應 3 1.2.2 選擇性觸媒還原反應之機制 3 1.3 觸媒介紹 4 1.3.1 應用於選擇性觸媒還原反應之觸媒 4 1.3.2 氧化鈰觸媒應用於選擇性觸媒還原反應 6 1.3.3 以硫化活化氧化鈰之選擇性觸媒還原反應 7 1.3.4 二氧化硫吸附於氧化鈰之表面化學 11 第二章 實驗方法 13 2.1 實驗藥品 13 2.2 觸媒製備-以二氧化硫氣體硫化氧化鈰觸媒 13 2.3催化反應 14 2.3.1 反應系統架設 14 2.3.2 氨氣選擇性觸媒還原反應測試 15 2.3.3 產物鑑定-質譜儀 16 2.4 觸媒鑑定 23 2.4.1 高解析電子微探儀 23 2.4.2 掃描式電子顯微鏡 23 2.4.3 X光繞射儀 23 2.4.4 比表面積及孔隙分布測定儀 24 2.4.5 拉曼光譜儀 26 2.4.6 熱重分析儀 26 2.4.7 氫氣程溫還原儀 27 2.4.8 X射線吸收光譜儀 28 2.5 反應機制鑑定 29 2.5.1 傅立葉轉換紅外線光譜儀 29 2.5.2 程序升溫脫附 30 第三章 結果與討論 31 3.1 反應活性結果 31 3.1.1 脫硝轉化率以及氮氣選擇率結果 31 3.1.2 反應穩定性測試 33 3.2 觸媒鑑定結果 35 3.2.1 觸媒元素組成比例 35 3.2.2 觸媒表面形貌 36 3.2.3 觸媒晶型結構 37 3.2.4 觸媒比表面積與孔徑分佈 40 3.2.5 觸媒硫化物含量分析 41 3.2.6 觸媒硫元素配位狀態分析 42 3.2.7 觸媒氧空缺之分析 44 3.2.8 觸媒還原性質之分析 46 3.2.9 觸媒硫化物種類分析 48 3.3 反應機制探討 53 3.3.1 氨氣於觸媒表面上之吸附行為 53 3.3.2 一氧化氮於觸媒表面上之吸附行為 58 3.3.2 選擇性脫硝還原之反應機制 62 第四章 結論 69 第五章 未來展望與建議 70 附錄 71 參考文獻 75 個人簡歷 80 | |
| dc.language.iso | zh-TW | |
| dc.title | 氧化鈰觸媒的硫化前處理及氨氣選擇性脫硝還原反應 | zh_TW |
| dc.title | Ceria Catalyst: Sulfurization Pretreatment and Selective Catalytic Reduction of Nitric Oxide with Ammonia | en |
| dc.date.schoolyear | 109-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 吳紀聖(Hsin-Tsai Liu),魏銘彥(Chih-Yang Tseng) | |
| dc.subject.keyword | 氧化鈰觸媒,氮氧化物,脫硝技術,選擇性觸媒還原反應,酸性位點,硫化處理,原位擴散反射傅立葉轉換紅外線光譜, | zh_TW |
| dc.subject.keyword | CeO2 catalyst,NOx removal,selective catalytic reduction,sulfurization treatment,acid site,in-situ IR, | en |
| dc.relation.page | 80 | |
| dc.identifier.doi | 10.6342/NTU202103062 | |
| dc.rights.note | 同意授權(全球公開) | |
| dc.date.accepted | 2021-09-30 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
| dc.date.embargo-lift | 2026-09-26 | - |
| 顯示於系所單位： | 化學工程學系 | |
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