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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 萬本儒(Bez-Zu Wan) | |
dc.contributor.author | Yan-Ru Lin | en |
dc.contributor.author | 林延儒 | zh_TW |
dc.date.accessioned | 2021-06-08T07:26:00Z | - |
dc.date.copyright | 2008-07-21 | |
dc.date.issued | 2008 | |
dc.date.submitted | 2008-07-14 | |
dc.identifier.citation | [1] C. S. Song, “Fuel processing for low-temperature and high-temperature fuel cells - Challenges, and opportunities for sustainable development in the 21st century,” Catalysis Today, vol. 77, p. 17, Dec, 2002.
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/26795 | - |
dc.description.abstract | 本研究以沉澱沉積法製備Au/CeO2,期望製備在低溫(200℃)水氣轉移反應中,具有高CO轉化率之觸媒。嘗試研究如下變因:(1) 鹼液中處理CeO2表面的影響;(2)金溶液酸鹼度的影響;(3) Au/CeO2前處理的影響;(4)保存Au/CeO2的方式。研究中並對觸媒的活性變化作鑑定和探討,鑑定方式包括:AA、UV-Vis、HRTEM、XRD。
研究結果顯示以表面修飾至pH值為6到8的CeO2最為適合,未經表面修飾或是修飾至pH值為10的CeO2所製成的觸媒會造成轉化率些微的下降;金溶液則以調至pH值為9所製成的Au/CeO2效果最佳,因為此時可使氯化金酸中的氯離子完全被OH-取代;Au/CeO2若在200oC下經一氧化碳前處理,因能維持小的金顆粒而有較高的催化活性;最後,製備好的Au/CeO2需儲存於冰箱的冷凍庫中,以免發生活性衰退的情形。 應用較佳的Au/CeO2,在總體積流速33.33ml/min(298K),反應溫度200℃,及以下兩種進料莫耳比例:(1) CO/H2O/N2 = 2.65/41.17/56.18;(2) CO/H2O/H2/CO2= 2.65/41.17 /44.94/11.24,分別測試催化活性。在(1)條件中,CO轉化率達98%,已接近理論平衡轉化率;但在(2)條件中,轉化率僅約73%,顯示觸媒的催化活性在未來仍具改善的空間。 | zh_TW |
dc.description.abstract | The purpose of this research is to investigate Au/CeO2 which is prepared by deposition-precipitation method (DP method) with high CO conversion under low temperature water-gas-shift reaction (WGSR). Preparation factors listed below are studied: (1) CeO2 surface modification by NaOH(aq); (2) pH value of gold solution for deposition; (3) pretreatment of Au/CeO2 before water-gas-shift reaction; (4) Au/CeO2 storage effect. Additionally, the properties of the catalysts are characterized by AA, UV-Vis, HRTEM, XRD.
The experimental results indicate that CeO2 with surface modification to pH=6 ~ 8 possesse the better performance; however, the CO conversion would decrease when the CeO2 with surface modification to pH=10 or without surface modification. The better pH value for the gold solution for deposition is 9, because the four Cl- in the solution could be ideally replaced by OH-. Au/CeO2 pretreated before reaction by CO at 200oC has the best CO conversion, because of the smallest particle size of gold particles. Finally, Au/CeO2 needs to store under low temperature without light (i.e., in a refrigerator) to protect against decay. For the tests of water-gas-shift reaction, the total flow rate and reaction temperature were carried out at 33.33ml/min and 200℃. Two mole flow rate ratios at reactor inlet : (1)CO/H2O/N2 = 2.65/41.17/56.18;(2) CO/H2O/H2/CO2=2.65/41.17/ 44.94/11.24 were used. For the best performance Au/CeO2 catalyst prepared in this research, CO conversion of condition (1) was 98%, which is approaching the equilibrium conversion obtained from thermodynamics simulation; however, CO conversion of condition (2) could only reach 73%. This implies there is still much room to improve the performance of the catalyst in the future. | en |
dc.description.provenance | Made available in DSpace on 2021-06-08T07:26:00Z (GMT). No. of bitstreams: 1 ntu-97-R95524007-1.pdf: 2033908 bytes, checksum: 19a71366d5a7d733a75af0ab0d592746 (MD5) Previous issue date: 2008 | en |
dc.description.tableofcontents | 摘要 ..………………………………………………………………………… I
Abstract ..………………………………………………………………………….II 目錄 ..…………………………………………………………………………IV 圖索引 ..…………………………………………………………………………VI 表索引 IX 第一章 緒論 1 1.1 研究緣起 1 1.1.1 燃料電池(Fuel Cell) 1 1.1.2 水煤氣轉移反應(Water-Gas Shift Reaction或WGSR) 5 1.2 研究背景 9 1.3 研究目標 12 第二章 金觸媒文獻回顧 13 2.1 金觸媒之發展 13 2.2 影響金觸媒催化活性的變因 15 2.2.1 金觸媒的製備方式 15 2.2.2 擔體之選擇 19 2.2.3 金顆粒的粒徑大小 20 2.2.4 擔體與金顆粒間的接觸結構 21 2.2.5 總結 22 第三章 實驗方法 23 3.1 觸媒製備 23 3.1.1 實驗藥品 23 3.1.2 實驗儀器 24 3.1.3 擔體製備 24 3.1.4 觸媒製備程序 26 3.2 反應測試 28 3.2.1 反應氣體 28 3.2.2 反應裝置 29 3.3 觸媒鑑定 33 3.3.1 原子吸收光譜 (AA) 33 3.3.2 X光粉末繞射儀(XRD) 34 3.3.3 紫外光可見光光譜儀 (UV-Vis) 35 3.3.4 高解析穿透式電子顯微鏡 (HRTEM) 36 3.4 金觸媒的儲存 36 3.5 定義與理論計算 37 3.5.1 氯離子置換率與pH值 37 3.5.2 轉化率 39 3.5.2.1 轉化率定義 39 3.5.2.2 平衡常數的計算 40 3.5.2.3 理論平衡轉化率 43 第四章 結果與討論 46 4.1 Au/CeO2對WGSR影響 46 4.1.1 擔體效應 47 4.1.2 金溶液酸鹼性效應 52 4.1.3 前處理效應 55 4.1.4 儲存溫度的影響 57 4.2 Au/CeO2鑑定 60 4.2.1 AA鑑定結果與討論 60 4.2.2 UV-Vis鑑定結果與討論 61 4.2.2.1 前處理效應 63 4.2.2.2 金溶液酸鹼性效應 67 4.2.2.3 儲存溫度的影響 68 4.2.2.4 結論 69 4.2.3 HRTEM鑑定結果與討論 71 4.2.4 XRD鑑定結果與討論 75 4.3 綜合討論 80 4.3.1 金顆粒粒徑大小 80 4.3.1.1 前處理效應 80 4.3.1.2 氯離子置換率 83 4.3.2 活性差異 85 4.3.3 不同的前處理比較 88 第五章 結論 89 第六章 未來展望 90 參考文獻 91 | |
dc.language.iso | zh-TW | |
dc.title | Au/CeO2觸媒在水氣轉移反應上的應用 | zh_TW |
dc.title | Application of Au/CeO2 over Water-Gas Shift Reaction | en |
dc.type | Thesis | |
dc.date.schoolyear | 96-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 吳紀聖,劉端祺(Tuan-Chi Liu) | |
dc.subject.keyword | 低溫水氣轉移反應,金觸媒,二氧化鈰,金溶液酸鹼度,金顆粒粒徑大小,前處理,儲存溫度, | zh_TW |
dc.subject.keyword | low temperature water-gas-shift reaction(WGSR),gold catalysts,CeO2,pH of gold solution,particle size of gold particles,pretreatment,storage effect, | en |
dc.relation.page | 94 | |
dc.rights.note | 未授權 | |
dc.date.accepted | 2008-07-14 | |
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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