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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 萬本儒(Ben-Zu Wan) | |
dc.contributor.author | Yu-Hsiang Huang | en |
dc.contributor.author | 黃昱翔 | zh_TW |
dc.date.accessioned | 2021-06-17T04:31:58Z | - |
dc.date.available | 2020-08-20 | |
dc.date.copyright | 2018-08-20 | |
dc.date.issued | 2018 | |
dc.date.submitted | 2018-08-10 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/70592 | - |
dc.description.abstract | 本研究利用沉積沉澱法將四氯金酸擔載於不同表面電位之二氧化鈦上,應用在常溫一氧化碳氧化反應。觸媒相關物化性質是由AA、HRTEM、XPS、XRD與Zeta Potential Analyzer等儀器鑑定。
Au/TiO2以四氯金酸做為前驅物,研究中控制金溶液之pH值來改變二氧化鈦擔體的表面電位,以探討對金負載量、奈米金催化活性、表面金的價態以及氯殘留量的影響。研究發現,未調整pH值之金溶液其pH值(e.g., pH=2.6)本來就低於二氧化鈦的等電位點(pH=7.5) ,直接使用就能使二氧化鈦表面電位為正,與溶液中帶負電的金前驅物(四氯金酸)有強烈庫侖吸引力,使金物種較容易的擔載在二氧化鈦上。由於殘留的氯離子會降低金觸媒活性,沉澱沉積程序後會以氫氧化鈉鹼液滴定將負載金觸媒之擔體懸浮液從pH 2.6調整至6,以置換觸媒上的氯離子為氫氧離子。然而本研究發現,強烈庫侖吸引力仍會使部份的氯離子無法被置換出來,使表面的金偏向氧化態,降低金觸媒的催化活性。若是在沉澱沉積前事先將金溶液以氫氧化鈉鹼液滴定,將pH值(pH=2.6)調整為6,然後才加入二氧化鈦進行沉澱沉積程序。研究結果發現雖然二氧化鈦表面在pH 6環境下已接近等電位點(較不帶電使庫侖吸引力較弱),致使金負載量較低,但是懸浮液中之金前驅物(四氯金酸)的氯在擔載前就已能有效被置換,因而降低二氧化鈦奈米金觸媒中氯的殘留,而能提高觸媒的催化活性及穩定性。本研究顯示二氧化鈦擔體表面電位以及沉澱沉積程序對奈米金觸媒有顯著影響,強烈庫侖吸引力利於沉澱沉積但不利於後處理程序中氯離子的置換。 研究中進一步討論製備程序對金觸媒反應活性的影響。觸媒製備程序中,金溶液調整後的pH值、載負溫度、去離子水洗及乾燥觸媒的方式等步驟是影響氯離子殘留、金顆粒載負和反應活性的主要製備變因,結果顯示,將金溶液調整pH值為6,並於80°C的溫度下進行沉積沉澱的程序,並經過60°C攪拌水洗的方式,最後於60°C飽和水蒸汽環境乾燥,能有效去除殘留在觸媒的氯離子,提升反應活性。 | zh_TW |
dc.description.abstract | In this research, tetrachloroauric acid was loaded on titania with different zeta potentials by deposition-precipitation method and applied for carbon monoxide oxidation at room temperature. The properties of the catalysts were characterized by using various instruments such as AA, HRTEM, XPS, XRD and Zeta Potential Analyzer.
Tetrachloroauric acid was used as a precursor for Au/TiO2. The pH of the gold solution was controlled to change the zeta potential of the titania, for investigating the effects on gold loading, the catalytic activity, the valence states of surface gold, and residual chlorine. It was found that pH of an unadjusted gold solution (e.g., pH=2.6) was much lower than the isoelectric point (IEP) of titania (pH=7.5), so that the surface potential of titania was positive when used directly. The Coulomb force resulted from the negatively charged gold precursor (tetrachloroauric acid) and the positively charged titania support was strong. Therefore, 86% gold in the solution can be deposited onto titania. Since the residual chloride ions decrease the activity of the gold catalyst, the suspension was adjusted from pH 2.6 to 6 after the deposition, by dropwise addition of sodium hydroxide in order to displace the chloride ions on the catalyst. However, it was found that the strong Coulomb force caused some of the chloride ions remained, resulting in substantial gold oxides on the surface and decreasing the catalytic activity. If the gold solution was previously titrated with sodium hydroxide before deposition process, meaning the pH was adjusted from 2.6 to 6 before titania was added to the solution for the deposition. The results confirm the lower gold loading, because the surface charge of titania is close to neutral and the weaker Coulomb force. However, chlorine ions can be effectively replaced before the deposition, thereby reducing the residual chlorine remaining on the catalysts, resulting in higher catalytic activity and higher stability. This study has shown that the zeta potential of titania support and Coulomb force in deposition-precipitation procedures have significant impacts on nano-gold catalyst. Coulomb force favors the deposition of gold but does not favor for the replacement of chloride ions in the post-treatment process. In the research, influence of preparation procedures on catalytic activity of Au/TiO2 were further studied. The effects of deposit temperature, the ways of washing, and the methods of drying for Au/TiO2 were investigated. It has been concluded that the gold solution adjusted to pH 6 for the deposition at 80°C,the filter cake washed in water at 60°C, and the solid dried in a saturated vapor atmosphere at 60°C, can effectively increase the catalytic activity of Au/TiO2 for CO oxidation. | en |
dc.description.provenance | Made available in DSpace on 2021-06-17T04:31:58Z (GMT). No. of bitstreams: 1 ntu-107-R05524024-1.pdf: 2746401 bytes, checksum: fdc95cdbccc03ea4de526cf8a7c609d0 (MD5) Previous issue date: 2018 | en |
dc.description.tableofcontents | 口試委員審定書
致謝 摘要 I Abstract III 目錄 V 圖目錄 VII 表目錄 X 第一章 緒論 1 1.1. 研究背景 1 1.1.1 CO對人體毒害 1 1.1.2 三項觸媒轉化器中CO的移除 2 1.1.3 燃料電池中CO的移除 5 1.2. 常用觸媒介紹 7 1.3. 研究目標 13 第二章 文獻回顧 14 2.1 一氧化碳氧化反應機制 14 2.2 影響金觸媒活性的因素 15 2.2.1. 觸媒製備方式 16 2.2.2. 金擔載量 21 2.2.3. 顆粒粒徑的影響 23 2.2.4. 擔體的選擇 25 2.3 金觸媒於CO 氧化反應 29 2.3.1. 氯離子對金觸媒於CO 氧化反應之影響 29 2.3.2. 水氣對金觸媒於CO 氧化反應之影響 29 2.4 總結 32 第三章 實驗方法 35 3.1 觸媒製備 35 3.1.1. 實驗藥品 35 3.1.2. 實驗儀器 36 3.1.3. 觸媒製備程序 36 3.2 觸媒鑑定 40 3.2.1. 原子吸收光譜 (AA) 40 3.2.2. 界面電位分析儀(Zeta Potential Analyzer) 41 3.2.3. 高解析穿透式電子顯微鏡 (HRTEM) 42 3.2.4. X射線光電子光譜(XPS) 42 3.2.5. 能量色散X射線光譜(EDS) 43 3.2.6. X射線繞射分析(XRD) 44 3.3 觸媒活性測試 45 3.3.1 反應氣體 47 3.3.2 反應裝置 47 3.4 定義及理論計算 48 3.4.1 氯離子置換率 48 第四章 結果與討論 50 4.1. 表面電位對金觸媒擔載的研究 50 4.1.1. Au/TiO2的金擔載量分析 50 4.1.2. Au/TiO2的活性分析 52 4.1.3. Au/TiO2的金顆粒的探討 53 4.1.4. Au/TiO2的金表面型態的分析 55 4.1.5. Au/TiO2金觸媒結構分析 57 4.1.6. Au/TiO2氯殘留量分析 58 4.1.7. 不同擔體(TiO2及Y)結果討論 62 4.2. 探討金觸媒製備程序研究 67 4.2.1. 飽和水蒸汽乾燥 67 4.2.2. 擔載溫度影響 72 4.2.3. 擔載pH值影響 73 4.2.4. 水洗方式的影響 77 4.3. 反應條件研究 78 4.3.1. 熱傳對反應活性的影響 78 4.3.2. 水氣對反應機制的影響 79 第五章 結論 81 第六章 未來展望與建議 81 第七章 參考文獻 82 | |
dc.language.iso | zh-TW | |
dc.title | 表面電位於金/二氧化鈦製備程序對催化一氧化碳氧化之影響 | zh_TW |
dc.title | Preparation of Au/TiO2 for CO Oxidation: Surface Charge Effect | en |
dc.type | Thesis | |
dc.date.schoolyear | 106-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 鄭淑芬(Soo-fin Cheng),游文岳(Wen-Yueh Yu) | |
dc.subject.keyword | 奈米金觸媒,二氧化鈦,表面電位,氯,製備程序,一氧化碳氧化反應, | zh_TW |
dc.subject.keyword | nano-gold,titania,zeta potential,chlorine,preparation procedure,CO oxidation, | en |
dc.relation.page | 87 | |
dc.identifier.doi | 10.6342/NTU201802987 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2018-08-13 | |
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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ntu-107-1.pdf 目前未授權公開取用 | 2.68 MB | Adobe PDF |
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