利用還原劑與觸媒搭配將廢氣中的NOx還原成N2的技術可依反應特性分為選擇性觸媒還原法(Selective Catalytic Reduction, SCR)與非選擇性觸媒還原法(Non-Selective Catalytic Reduction, NSCR) 兩大類。 若觸媒能使還原劑與NO反應的速率遠大於還原劑與O2反應的速率，則還原劑只針對NOX反應而稱為SCR反應系統。反之，在NSCR系統中因觸媒無法使兩個競爭反應的速率有足夠的差異，故它們會同時進行，甚至必須先將O2消耗殆盡才能使NO明顯去除。
以氨(Ammonia, NH3)為還原劑的SCR (簡稱NH3-SCR)為現今處理鍋爐及柴油引擎廢氣中的NOx的主流技術。然而，此法常用的V2O5觸媒和沸石觸媒有起始反應溫度(Starting Reaction Temperature, SRT)偏高的缺點，昂貴的白金觸媒的溫度需求雖然較低，卻有反應溫度區間狹窄的問題。此外，NH3-SCR一直都存在著觸媒易受SO2中毒的困擾以及過剩的NH3可能衍生PM2.5污染的疑慮。NSCR主要用於汽油引擎的廢氣處理，只有零星的工業使用案例。由於汽油引擎為貧氧燃燒，廢氣中能扮演還原劑角色的碳氫化合物(HC)以及CO在數量上足夠將O2用盡並且去除NOx。這種應用方式通常屬於三效觸媒轉化器(Three Way Catalytic Convertor)的一部分，目前大多使用銠(Rh)為觸媒，其成本頗高。
本研究企圖使用成本較低之鐵氧磁體觸媒(Ferrite Catalyst)來降低NOx的處理成本，並且以H2作為還原劑來避免過剩的NH3或HC發生二次污染的可能性。實驗結果指出銅鐵氧磁體(Cu-ferrite)去除NO的效果優於其他鐵氧磁體。 Cu/Fe=1/2.5的Cu-ferrite具有最佳的催化效果，在含氧量0.3%的條件下，180ºC以下就能啟動反應，且只需220ºC就能達到90%之轉化率。更進一步的測試發現， H2分別與NO和O2所進行的反應彼此競爭，在不同的觸媒作用下呈現多種樣貌，可用以深入解析SCR與NSCR之機制。
另一方面，為貼近實務狀況而作的幾個模擬試驗證明了即使有高濃度的SO2存在也不會造成Cu-ferrite觸媒中毒，這對於含硫燃料燃燒後的廢氣處理而言是一項極大的優點。

According to the reaction characteristics, the technique of reducing NOx in the exhaust gas to N2 by using a reductant and a catalyst can be divided into two categories: Selective Catalytic Reduction (SCR) and non-selective Catalytic Reduction (NSCR).
That is referred to SCR reaction system if the catalyst is capable of reacting the reductant with NO much faster than the rate at which the reductant reacts with O2, the reductant only for the reaction of reducing NOX. Conversely, in the NSCR system, because the catalyst cannot make enough difference between the rates of the two competitive reactions, they will proceed simultaneously, and even need to exhaust the oxygen before NO can be removed significantly.
NH3-SCR, the SCR with ammonia (NH3) as a reductant is the main technology to treat NOx in exhaust of boilers and diesel engines nowadays. However, the V2O5 catalyst and zeolite catalyst commonly used in this method have the disadvantage of high initial reaction temperature (SRT). Although the temperature requirement of expensive platinum catalysts is low, there is a problem that the reaction temperature range is narrow. In addition, NH3-SCR has always been concerned that the catalyst is susceptible to SO2 poisoning and the suspicion that excess NH3 may cause PM2.5 contamination.
NSCR is mainly used for the exhaust gas treatment of gasoline engines, and there are only sporadic cases for industrial use. Owing to oxygen-lean combustion in gasoline engines, hydrocarbons (HC) and CO in exhaust gases, which can act as reductants, are sufficient in quantity to exhaust O2 and remove NOx. This application is usually part of the three way catalytic convertor. Rh is mostly used as catalyst at present, and its cost is quite high.
The purpose of this study is to reduce the cost of NOx treatment by using inexpensive ferrite catalyst, and use H2 as a reductant to avoid the possibility of secondary pollution of excess NH3 or HC. The experimental results indicate that Cu-ferrite is better than other ferrites in removing NO. Cu-ferrite with Cu/Fe=1/2.5 has the best catalytic effect. Under the condition of 0.3% oxygen content, the reaction can be started below 180ºC, and 90% conversion can be achieved at 215ºC. Further tests found that O2 competes with NO to react with H2, and presents various appearances under different catalysts, which can be used to deeply analyze the mechanism of SCR and NSCR.
On the other hand, several simulated experiments to close to the actual situation have proved that even the presence of high concentration of SO2 will not cause the poisoning of Cu-ferrite catalyst, which is a great advantage for waste gas treatment after combustion of sulfur-containing fuels.

摘要 i
Abstract iii
致謝 v
目錄 vi
表目錄 ix
圖目錄 x
第一章 緒論 1
1-1 研究背景 1
1-2 研究綱要 3
第二章 文獻回顧 4
2-1 氮氧化物的主要來源 4
2-2 氮氧化物的簡介與危害 5
2-3 氮氧化物的形成 9
2-4 氮氧化物處理技術 11
2-5 SCR與NSCR之觸媒選擇 14
2-6 常見之SCR與NSCR系統 17
2-7 SCR與NSCR系統中氧氣濃度影響 20
2-8 觸媒成型技術 23
2-8-1 蜂巢型 24
2-8-2 平板型觸媒 25
2-8-3 其他類型的觸媒 25
2-9鐵氧磁體程序法 26
2-9-1 鐵氧磁體特性 29
2-9-2 鐵氧磁體之應用 29
2-10 觸媒催化反應 31
2-11 觸媒中毒 33
2-12 過剩還原劑排放造成二次汙染 34
2-13 相關文獻回顧 35
第三章 研究方法及實驗設備 38
3-1 研究方法 38
3-1-1 研究規劃 38
3-1-2 研究方法 39
3-2 實驗藥品及設備 44
3-2-1實驗設備 44
3-2-2試藥及氣體 46
第四章 結果與討論 49
4-1 觸媒篩選 49
4-2 NO與O2間的反應關係 54
4-3 高濃度SO2對於銅鐵氧磁體觸媒中毒之影響 64
第五章 結論 68
參考文獻 70

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