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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 劉雅瑄(Ya-Hsuan Liou) | |
| dc.contributor.author | Wen-Ta Yang | en |
| dc.contributor.author | 楊汶達 | zh_TW |
| dc.date.accessioned | 2022-11-25T06:33:50Z | - |
| dc.date.copyright | 2022-02-21 | |
| dc.date.issued | 2022 | |
| dc.date.submitted | 2022-02-14 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/82216 | - |
| dc.description.abstract | "本研究以一步驟氣溶膠輔助自組裝法製備高分散性之銅/二氧化鈦微米球(CuTMS)進行熱催化氧化去除一氧化碳，並結合原位分析技術深入了解其催化氧化反應機制。催化氧化一氧化碳反應利用在線式質譜儀監測銅/二氧化鈦微米球對一氧化碳的去除能力與反應溫度間的關係性，發現於相對高摻雜比例的銅/二氧化鈦觸媒對一氧化碳具有完全去除的能力，最低僅需約160℃即可。而長時間(200小時)的連續催化反應以及三次迴圈重複實驗結果中，CuTMS仍以高度的穩定性進行反應。X射線光電子能譜（XPS）分析中指出所製備的觸媒隨著銅摻雜而產生 Ti（III）的存在，可能形成Cu–O–Ti 結構；並利用一氧化二氮(N2O)輔助氫氣程溫還原法量測，計算得知銅摻雜的表面分散度可高達80%、粒徑僅約1.2 nm及銅的暴露表面積可達550 m2/gCu；並且結合原位傅里葉變換紅外光譜（in-situ FTIR）分析，觀察到2080 , 2130 與2360 cm-1處具有明顯的吸收峰，分別對應到銅對CO的吸附與CO2的吸附。從上述研究結果結合一氧化碳催化氧化的週轉頻率計算，歸納出銅/二氧化鈦觸媒同時具備有由銅入侵二氧化鈦結構中的Cu–O–Ti結構以及過量銅添加所析出於二氧化鈦表面的銅氧化物團簇兩種活性位置，其中Cu–O–Ti主導整體的一氧化碳催化氧化反應，而在富氧環境中表面的銅則在≤ 70℃的反應溫度就能進行催化反應。除了催化反應的活性位置外，我們經由一氧化碳的程溫還原串聯氧氣的程溫氧化反應，觀察所製備的銅/二氧化鈦觸媒催化氧化一氧化碳的氧氣供給以及補給行為，發現在缺氧環境中Cu–O–Ti可以提供自身的晶格氧使一氧化碳氧化成為二氧化碳，緊接著在氧氣的程溫氧化反應中，我們觀察到了氧氣得補給行為。為研究反應中晶格氧的失去以及補給，我們導入了operando Raman光譜，通過顯微反應器的輔助，觀察到在較低的反應溫度下一氧化碳會先吸附於催化劑表面，當反應溫度上升的過程中通過活性位置的作用使表面吸附的碳酸鹽物種去除，防止催化劑的積碳或是毒化行為的發生，同時亦證實了二氧化鈦的結構隨著反應溫度的上升，出現了明顯的結構變化所產生的缺陷，並且隨著反應溫度的下降逐步恢復到與反應前相似的狀態。 因此這種由Cu–O–Ti結構主導對一氧化碳催化氧化的反應活性，其反應過程中氧的失去而產生氧空缺，而氧空缺的補給使其再次氧化，周而復始使得催化反應不斷延續不至於降低活性，此類型的反應屬於Mars-van Krevelen型態的反應機制。而本研究結果將有助於未來的一氧化碳催化氧化觸媒的研發以及催化反應機制的相關後續研究，藉以降低可能的空氣污染行為以及保障的人類生命財產安全。 " | zh_TW |
| dc.description.provenance | Made available in DSpace on 2022-11-25T06:33:50Z (GMT). No. of bitstreams: 1 U0001-2401202216044300.pdf: 10426073 bytes, checksum: c1258e4279092df1b5373697adf39f90 (MD5) Previous issue date: 2022 | en |
| dc.description.tableofcontents | 謝辭 I 摘要 II Abstract IV 圖目錄 VIII 表目錄 X 第一章、緒論 1 1.1 研究緣起 1 1.2 研究目的 2 1.3 研究內容 2 Chapter 2. 第二章、文獻回顧 4 2.1 一氧化碳議題 4 2.1.1 一氧化碳 4 2.1.2 生物毒性 5 2.1.3 一氧化碳的來源與影響 6 2.2 一氧化碳的處理技術 13 2.3 材料選擇 14 2.3.1 材料製備方法 14 2.3.2 催化材料的選定 15 2.4 一氧化碳催化氧化機制 16 2.5 Operando原位動態技術 17 Chapter 3. 第三章、材料製備與實驗方法 20 3.1 實驗內容與架構 20 3.2 材料製備 20 3.3 實驗儀器與方法 21 3.3.1 材料特性分析 22 3.3.2 化學性質鑑定 26 3.3.3 原位分析技術 28 Chapter 4. 第四章、活性位置作用評估 29 4.1 CuTMS表面形貌與特性分析 29 4.2 一氧化碳催化氧化反應與穩定性分析 39 4.3 原位傅立葉紅外光光譜分析 41 4.4 銅活化位的作用 44 4.5 小結 50 Chapter 5. 第五章、Operando催化反應動態解析 52 5.1 一氧化碳催化氧化的遲滯行為模式 52 5.2 氧的供給與補給行為觀察 59 5.3 材料的結構缺陷評估 64 5.4 小結 72 Chapter 6. 第六章、結論與建議 74 6.1 結論 74 6.2 建議 75 參考文獻 76 附錄 95 | |
| dc.language.iso | zh-TW | |
| dc.subject | 原位傅里葉紅外光譜 | zh_TW |
| dc.subject | 一氧化碳催化氧化 | zh_TW |
| dc.subject | 原位動態拉曼光譜 | zh_TW |
| dc.subject | 氣溶膠輔助自組裝法 | zh_TW |
| dc.subject | 銅-二氧化鈦微米球 | zh_TW |
| dc.subject | operando Raman | en |
| dc.subject | catalytic CO oxidation | en |
| dc.subject | one-step AASA | en |
| dc.subject | Cu/TiO2 mesospheres | en |
| dc.subject | in-situ FTIR | en |
| dc.title | 原位動態拉曼解析銅摻雜二氧化鈦中孔微米球催化氧化一氧化碳反應之研究 | zh_TW |
| dc.title | Operando Raman Analysis on Copper Doped TiO2 MesoporousMicrosphere for CO Catalytic Oxidation | en |
| dc.date.schoolyear | 110-1 | |
| dc.description.degree | 博士 | |
| dc.contributor.author-orcid | 0000-0002-7339-3955 | |
| dc.contributor.oralexamcommittee | 胡景堯(Daniel Fu-Chang Tsai),林進榮(Hsin-Ju Kuo),董崇禮,官文惠 | |
| dc.subject.keyword | 銅-二氧化鈦微米球,氣溶膠輔助自組裝法,一氧化碳催化氧化,原位傅里葉紅外光譜,原位動態拉曼光譜, | zh_TW |
| dc.subject.keyword | Cu/TiO2 mesospheres,one-step AASA,catalytic CO oxidation,in-situ FTIR,operando Raman, | en |
| dc.relation.page | 102 | |
| dc.identifier.doi | 10.6342/NTU202200179 | |
| dc.rights.note | 未授權 | |
| dc.date.accepted | 2022-02-14 | |
| dc.contributor.author-college | 理學院 | zh_TW |
| dc.contributor.author-dept | 地質科學研究所 | zh_TW |
| dc.date.embargo-lift | 2027-02-11 | - |
| 顯示於系所單位： | 地質科學系 | |
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