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姓名	陳俊翔(Jun-Xiang Chen)  查詢紙本館藏	畢業系所	環境工程研究所
論文名稱	結合錳基觸媒及非熱電漿技術提升SCR活性之研究 (Combining nonthermal plasma with Mn-based catalyst for higher SCR activity)
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摘要(中)	氮氧化物(NOx)排放及其衍生之二次污染已成為全球重要的空氣汙染問題，對人體健康及環境造成深遠的影響，包含酸雨、光化學煙霧、水體品質、能見度降低及人體呼吸系統疾病等。於去除氮氧化物技術中，以SCR技術具有高轉化效率，但典型之SCR觸媒卻只在250~400oC溫度區間有好的轉化效果，於較低溫度下，無法有效轉化NOx，因此仍有改善空間。本研究以錳觸媒為基底，旨在探討於低溫條件對NO之去除效率，並結合非熱電漿進一步使錳基觸媒行fast-SCR反應以提升NO轉化效率。 本研究分為兩主軸，其一為利用含浸法製備錳基觸媒，並以Ce、Ni和Cu金屬改質觸媒活性相，分別製備10 wt.% MnCe/TiO2、10 wt.% MnCeNi/TiO2及10 wt.% MnCeCu/TiO2等三種觸媒，比較三種觸媒之活性與基本物化特性，並藉由操作參數瞭解觸媒的適用性。研究結果顯示10 wt.% MnCeNi/TiO2觸媒可於150oC達100% NO轉化效率，而10% wt. MnCe/TiO2及10% wt. MnCeCu/TiO2則需200oC才可將NO完全轉化，因此以10% wt. MnCeNi/TiO2觸媒進行後續實驗。其二為使用非熱電漿進行氣體組成調整，使氣流中之NO及NO2濃度略等量，以達fast-SCR反應條件，結果顯示於15.5 kV和10kHz之操作條件可使氣流中300 ppm NO有效轉化成165 ppm NO及153 ppm NO2，並於電漿系統下游端串接10 wt.% MnCeNi/TiO2觸媒，於100oC即可有效將NO完全轉化。在同時含有CO、CO2、C2H4、水氣及二氧化硫的氣體組成，可藉由電漿觸媒系統於100oC達90%NO轉化效率，整體而言，非熱電漿結合本研究改質之錳基觸媒具有於低溫下有效還原氮氧化物之效果，具實際應用潛力。
摘要(英)	Nitrogen oxides (NOx) has been regarded as one of the most serious air pollutants. It not only causes adverse environmental effects such as acid rain, photochemical smog, deterioration of visibility and water quality, but also harms human respiratory system. Among de-NOx technologies, selective catalytic reduction (SCR) is considered as the best control technology for NOx removal. However, SCR typically needs to be operated at a temperature window ranging from 250 to 400oC. If the system is operated at lower temperatures, NOx could not be reduced effectively. The aim of this study is to develop a low-temperature de-NOx technique via plasma catalysis and fast-SCR for effective NO reduction. This study could be divided into 2 aspects: (1) Mn-catalysts modified (including 10 wt.% MnCe/TiO2, 10 wt.% MnCeNi/TiO2 and 10 wt.% MnCeCu/TiO2) for de-NOx, (2) combining plasma catalysis and fest-SCR for de-NOx. Experimental results indicate that NO conversion achieved with 10 wt.% MnCeNi/TiO2 reaches 100% at 150oC, while 10 wt.% MnCe/TiO2 and 10 wt.% MnCeCu/TiO2 need to be operated at ?200oC for complete conversion. MnCeNi/TiO2 is further applied for plasma catalysis system due to its higher activities. Results indicate that 300 ppm NO could be converted into 165 ppm NO and 153 ppm NO2 with the applied voltage of 15.5 kV and frequency of 10 kHz and 100% NO conversion is achieved at 100oC by fast-SCR. Moreover, NO conversion still maintains 90% at 100oC with plasma catalysis system as CO, CO2, C2H4, SO2 and H2O(g) are introduced into the stream gas simultaneously. Overall, this study demonstrates that combining nonthermal plasma with Mn-based catalyst is effective in reducing NOx emission at a low temperature and has good potential for industrial application.
關鍵字(中)	★ 氮氧化物 ★ 選擇性觸媒還原法 ★ 非熱電漿 ★ 電漿催化	關鍵字(英)	★ NOx ★ SCR ★ nonthermal plasma ★ plasma catalysis
論文目次	中文摘要 I Abstract II 目錄 III 圖目錄 VI 表目錄 VIII 第一章 前言 1 1.1 研究緣起 1 1.2 研究目的 3 第二章 文獻回顧 5 2.1 氮氧化物之特性、危害及污染源 5 2.1.1. 氮氧化物之基本特性 5 2.1.2. 氮氧化物來源 7 2.1.3. 氮氧化物造成之危害 7 2.2 氮氧化物生成機制 9 2.3 氮氧化物控制技術 13 2.3.1. 燃燒前處理 (Precombustion Treatment) 13 2.3.2. 燃燒程序修正 (Combustion Modification) 13 2.3.3. 燃燒後處理 (Post Combustion Removal ) 16 2.4 選擇性觸媒還原法(SCR) 19 2.4.1. SCR介紹 19 2.4.2. SCR商業化觸媒 21 2.4.3. 低溫SCR觸媒 22 2.4.4. 觸媒表面之酸位基 27 2.4.5. SCR應用於柴油引擎排氣處理 28 2.5 Fast-SCR 30 2.6 反應動力探討 32 2.6.1. 觸媒異相反應模式 32 2.6.2. Arrhenius 方程式 33 2.7 電漿 34 2.7.1. 電漿簡介與其生成原理 34 2.7.2. 電漿性質與種類 36 2.7.3. 雙階段NTP結合觸媒之SCR反應 41 2.8 文獻總結 45 第三章 研究方法與設備 47 3.1 研究流程與架構 47 3.2 預備實驗 49 3.2.1. 觸媒製備 49 3.2.2. 觸媒材料之物化特性分析 50 3.3 實驗系統 54 3.4 實驗分析方法 56 3.4.1. 反應器 56 3.4.2. 實驗藥品與氣體 57 3.4.3. 分析系統 58 3.5 研究方法 60 3.6 實驗結果之計算 64 第四章 結果與討論 65 4.1 觸媒物化特性 65 4.1.1. BET氮氣吸脫附測試 65 4.1.2. XRD晶相分析 66 4.1.3. FE-SEM分析 66 4.1.4. SEM-EDS 元素分析 67 4.1.5. ESCA (XPS) 特性分析 68 4.1.6. H2-TPR 72 4.1.7. TGA之分析 73 4.2 Mn-based catalyst 測試 75 4.2.1. 溫度對於SCR反應之影響 75 4.2.2. 氧含量對於SCR反應之影響 76 4.2.3. 空間流速對SCR反應之變化 77 4.2.4. 觸媒之長效性測試 78 4.2.5. 水氣與二氧化硫對觸媒之影響 79 4.3 觸媒之動力分析 81 4.4 電漿輔助系統 84 4.4.1. 電漿輔助之SCR成效 85 4.4.2. 放電電壓對NO2/NO比值之影響 89 4.4.3. 放電頻率對NO2/NO比值之影響 89 4.4.4. 不同氧氣含量對NO2/NO比值之影響 91 4.4.5. 不同NO入口濃度對電漿放電之影響 92 4.4.6. 不同進氣組成之影響 93 4.4.7. 模擬柴油引擎氣氛 99 第五章 結論與建議 102 5.1 結論 102 5.2 建議 103 參考文獻 104
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指導教授	張木彬(Moo-Been Chang)	審核日期	2017-1-20
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