改質SCR觸媒以應用於同時去除戴奧辛與NOx之研究

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林建平(Jian-Ping Lin) 查詢紙本館藏

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論文名稱

改質SCR觸媒以應用於同時去除戴奧辛與NOx之研究
(Modification of SCR catalyst for simultaneous removal of dioxin and NOx from gas streams)

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摘要(中)

選擇性觸媒還原程序應用於排氣中NOx之控制已行之有年，其催化反應活性主要由釩氧化物提供，操作於300到400oC方能達到高去除效率，相關研究也證實SCR觸媒對於戴奧辛有很好的去除效果。本研究探討應用自製SCR觸媒同時去除戴奧辛與NOx之效率，並進一步添加貴重金屬進行觸媒改質，藉由貴重金屬的高催化活性以提升對污染物之催化特性。另一方面同時尋找具備多重污染物去除潛力之貴重金屬進行改質，以落實多重污染物排放控制策略 (multipollutant emission control)。文獻證實Ru具高轉化活性，且成本相較於其他Pt、Pd貴重金屬低。故本研究以V2O5/TiO2觸媒為基礎，添加Ru金屬進行改質，並製備多種不同成分配比之觸媒，以獲取較佳之觸媒成分。研究結果指出戴奧辛類污染去除方面，V2O5/TiO2觸媒反應溫度由150oC提升至300oC對於戴奧辛去除效率有正面之影響。5wt%V2O5/ TiO2在反應溫度為150oC時，對PCB之去除部分仰賴觸媒吸附效果而未實際與觸媒進行反應，破壞效率為68.9%;當溫度提升至200oC時，效率始有顯著提升，其去除機制方達到以觸媒破壞為主要動力，破壞效率達94.6%。改質後Ru/5wt%V2O5/TiO2觸媒在溫度150oC時顯著提升PCB破壞效率。在NOx去除方面，NO轉換效率受NH3添加劑量之影響較為顯著，在NH3:NO為1.2時，5wt%V2O5/TiO2對NO之轉換效率隨操作溫度上升而有顯著提升，並在300oC達99%;在NH3:NO為1時，溫度操作在250oC達最高效率為73%，副產物量測方面，操作溫度由300oC上升至400oC開始有明顯N2O之生成，並進一步發現N2O生成可能由NH3氧化生成，而觸媒之釩氧化物成分越高也會提升N2O生成之趨勢。經改質後3wt%Ru/ 5wt%V2O5/TiO2在300oC和350oC發現有更高NO轉換效率分別為79.8%、88.5%，並且對於N2O之生成有抑制作用。

摘要(英)

Selective catalytic reduction (SCR) is a well-established and widely used process for the abatement of NOx present in waste gases from stationary sources. The catalytic activity is mainly provided by vanadium oxide and it has to be operated at a temperature range of 300oC-400oC to achieve high NOx removal efficiency. Previous study indicates that the SCR catalyst can also be applied for PCDD/Fs removal. This study investigated the self-made traditional SCR catalyst for simultaneous removal of dioxin and NOx from gas streams, and modified the catalyst for higher activity and multiple pollutant removal. Literature confirmed that Ru is of high activity and the cost is lower than other noble metals, such as Pt and Pd. In this study, V2O5/TiO2 is modified by adding Ru, with different percentages. Experimental results indicate that Ru/5wt%V2O5/TiO2 catalyst significantly improves dioxin destruction efficiency at 150oC. For the removal of NOx, the modified 3wt%Ru/5wt%V2O5/TiO2 achieved higher NO conversion efficiencies of 79.8%, and 88.5%, respectively, at 300oC and 350oC, and also reduced N2O formation.

關鍵字(中)

★ 多重污染物控制
★ 戴奧辛
★ NOx
★ SCR

關鍵字(英)

★ NOx
★ dioxin
★ SCR
★ multi-pollutant control

論文目次

第一章前言 1
1.1 研究緣起 1
1.2 研究目的與範疇 2
第二章文獻回顧 3
2.1 戴奧辛介紹 3
2.1.1 戴奧辛基本特性 3
2.1.2 戴奧辛類化合物之毒性當量 7
2.1.3 戴奧辛生成機制 9
2.2 戴奧辛現行控制技術 12
2.3 NOX介紹 16
2.3.1 NOx基本特性 16
2.3.2 NO生成機制 17
2.4 NOX現行控制技術 18
2.5 觸媒催化特性 22
2.5.1 觸媒催化之原理與反應機制 22
2.5.2 觸媒種類與特性的比較 24
2.6 觸媒去除污染物之應用 26
2.6.1 De-Dioxins觸媒 26
2.6.2 De-NOx觸媒 31
第三章研究方法與步驟 35
3.1 研究設計流程 35
3.2實驗設備及試藥 38
3.2.1 實驗藥品 38
3.2.2 實驗溶劑 39
3.2.3 實驗材料 39
3.2.4 實驗設備 40
3.3戴奧辛樣品分析 41
3.3.1 戴奧辛樣品前處理 41
3.3.2 GC/HR分析儀器條件設定 44
3.3.3 戴奧辛類多氯聯苯分析程序 50
3.4 NOX分析 61
3.4.1 FT-IR分析條件 61
3.5實驗設計 63
3.5.1 實驗模組建立 63
3.5.2 反應操作參數 65
3.5.3 V2O5/TiO2觸媒製備 66
3.6其他儀器原理 69
3.6.1 BET比表面積分析儀 (ASAP 2010) 69
3.6.2 X光繞射分析儀 (XRD) 69
3.6.3 掃描式電子顯微鏡分析（SEM） 70
3.6.4 能量分散光譜儀 (EDS) 71
第四章結果與討論 72
4.1觸媒基本特性 72
4.1.1 BET 72
4.1.2 SEM 73
4.1.3 EDS 75
4.1.4 XRD 76
4.2戴奧辛去除探討 78
4.2.1 戴奧辛入口濃度測………..……………………………………..78
4.2.2 擔體測試 80
4.2.3 溫度對於戴奧辛去除、破壞之差異 82
4.2.4 觸媒配比對於PCB去除、破壞之差異 84
4.3 NOX去除探討 85
4.3.1 NH3劑量影響 86
4.3.2 觸媒配比對NOx去除影響 88
4.3.3 NH3 slip之探討 91
4.3.4 NOx去除效率 92
4.4 觸媒改質 93
4.4.1 改質後基本特性分析 96
4.4.2 改質後之deDioxin探討 100
4.4.3 改質後之deNOx探討 104
4.4.3.1 不同操作條件之探討 107
4.5. 最佳操作條件 112
第五章、結論與建議 114
5.1 結論 114
5.2 建議 115
參考文獻 ……………………………………………………………......…..116

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指導教授

張木彬(Moo-Been Chang)

審核日期

2012-8-25

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