本研究嘗試以觸媒氧化法來處理一氧化氮，使用之觸媒為以含浸法（Impregnation）製備之載體銅觸媒，包括Cu/TiO2、Cu/Al2O3、Cu/SiO2。處理後之產物二氧化氮雖然毒性比一氧化氮還高，但是水溶性佳，以純水或鹼液即可將其完全吸收，達到去除氣相污染物的目的。
實驗探討的部份共分為：觸媒之篩選、操作參數之探討與反應動力之推求。在觸媒篩選方面，本實驗探討以三種銅離子來源（硝酸銅、醋酸銅、硫酸銅）與三種載體（TiO2、Al2O3、SiO2）配置成之觸媒活性大小作一比較，結果顯示以硝酸銅配置之Cu/TiO2處理效果較佳，且有較寬廣之溫度操作區間，並比較不同銅附載量得知，8wt.%是最經濟之量，所以本部份實驗結果顯示8wt.%之Cu/TiO2為最佳的選擇。
在操作參數探討方面，NO入口濃度的大小會對觸媒氧化效率造成影響，在入口濃度大於1000ppm時，濃度越高，轉化率會越低，而在入口濃度小於1000ppm時轉化率幾乎不隨入口濃度而變化。在空間速度的選擇方面，實驗結果顯示，空間速度為15000 hr-1，也就是空床停留時間約在0.24秒時為較經濟的操作條件。而在水氣的影響方面，高的絕對溼度確實會對反應造成抑制之效果，可是抑制的情形很輕微，所以本觸媒氧化反應亦適合在高濕度下操作。
最後一部份探討反應動力式，本實驗之反應動力以積分反應實驗法求取。可得到正、逆反應之活化能分別為15.8kcal/mole與25.9 kcal/mole。由預測值與實驗值之比對可得本模式適用條件為：NO入流濃度介於300-1000ppm，停留時間約在0.12-0.48之間，絕對濕度在4854-42475ppm。

The study of catalytic oxidation on the removal of NO was investigated over the Cu-catalysts . The Cu-catalysts , including Cu/TiO2 , Cu/Al2O3 and Cu/SiO2 , were prepared by impregnation method . Alougth NO2 , the product of this reaction , has higher toxicity than NO , but it might be removed completely by absorption with H2O or alkalinal solution for its high solubility .

The experiments can be divided into three parts , i.e. , the screen of test catalysts , the effect of operating factors on the conversion of NO and the kinetic model . In the first part , the activity of test catalysts , which were prepared by mixing three various sources of Cu-ions（i.e., Cu(NO3)2 , Cu(CH3COO)2 , and CuSO4）with three different types of support（i.e., TiO2 , Al2O3 , and SiO2）, and were compared in form of conversion on NO to find the best catalyst . The results show that the mixture Cu(NO3)2 / TiO2 has the good performance on the conversion of NO , and also has more wider operating in range of temperature . In order to find the optimal loading of Cu on Cu(NO3)2 / TiO2 , additional test of various dosage over the catalysts was conduct in series . It is found that 8wt.% of Cu loading on Cu(NO3)2 / TiO2 is the most economic dosage . Therefore , we select this type of Cu oxide as the best catalyst in the following work .

In the second part , the effect of NO inlet concentration , space velocity and humidity on the conversion of NO were performed . The results show that the conversion of NO decreases with the increasing of [NO]in when [NO]in is larger than 1000ppm；the conversion of NO is not changed with [NO]in when [NO]in is lower than 1000ppm . The better space velocity is 15000hr-1 , i.e.,the empty bed residence time is 0.24 second . The reaction on NO conversion would be restrained by higher humidity contenting in inlet gas stream , but the effect of inhibition on NO conversion is not significant .

Finally , the kinetics of the oxidation of NO over 8wt.% Cu(NO3)2 / TiO2 was obtained by integral method .It is found that the oxidations of NO can be described by first order reversible reaction and the observed activation energy are 15.8 kcal/mole（forward reaction）and 25.9 kcal/mole（backward reaction）, respectively . By comparing the conversion of predicted NO with the experimentals , we can find the suitable operation conditions in application of the kinetic model : the inlet concentration of NO in a range of 300-1000ppm , the empty-bed residence time ranging from 0.12-0.48 second , and the absolute humidity ranging from 4854 to 42475ppm .

謝誌…………………………………………………………I
中文摘要……………………………………………………II
英文摘要……………………………………………………IV
目錄…………………………………………………………VI
表目錄……………………………………………………VIII
圖目錄………………………………………………………X
符號說明…………………………………………………………XII

第一章、 前言………………………………………………1

1-1 研究緣起………………………………………………1
1-2 一氧化氮的特性………………………………………2
1-3 一氧化氮的生成與排放………………………………3
1-4 一氧化氮的控制技術…………………………………3
1-5 研究目的………………………………………………6

第二章、 文獻回顧………………………………………10

2-1 觸媒氧化法之原理與發展……………………………10
2-2 以觸媒氧化法處理一氧化氮之可行性評估…………11
2-3 觸媒之製備條件探討…………………………………12
2-3-1 觸媒的種類與特性比較…………………………12
2-3-2 銅離子來源對銅觸媒催化能力之影響…………13
2-3-3 銅離子附載量對催化能力之影響………………15
2-3-4 載體對觸媒活性之影響…………………………16
2-4 操作參數之探討………………………………………19
2-4-1 操作溫度…………………………………………19
2-4-2 空間速度…………………………………………21
2-4-3 NO進流濃度………………………………………21
2-4-4 水氣濃度…………………………………………22
2-5 反應動力之推求………………………………………22

第三章、 觸媒的製備與鑑定方法………………………27

3-1 觸媒的製備方法………………………………………27
3-2 觸媒的鑑定……………………………………………27
3-2-1 X射線繞射分析(XRD)…………………………27
3-2-2 比表面積測量(BET)……………………………29
3-2-3 掃描式電子顯微鏡與能量分散成分分析……30



第四章、 實驗設備與研究方法…………………………31

4-1 化學藥品………………………………………………31
4-2 實驗設備與分析儀器…………………………………32
4-2-1 實驗設備………………………………………32
4-2-2 分析儀器………………………………………34
4-3 設備操作與實驗步驟…………………………………35
4-3-1 設備操作………………………………………35
4-3-2 實驗步驟………………………………………35
4-4 實驗之設計……………………………………………37
4-4-1 觸媒之鑑定……………………………………37
4-4-2 觸媒之篩選……………………………………39
4-4-3 操作參數之探討………………………………40
4-4-4 反應動力之推求………………………………41

第五章、 結果與討論……………………………………45

5-1 觸媒之物性分析………………………………………45
5-1-1 BET比表面積測量……………………………45
5-1-2 XRD(X-射線繞射分析)………………………45
5-1-3 SEM掃描式電子顯微鏡與EDS成分分析……51
5-2 觸媒之篩選試驗…………………………………56
5-2-1 不同銅離子來源配置之銅觸媒活性比較…56
5-2-2 不同載體配置之銅觸媒活性比較…………60
5-2-3 銅附載量對銅觸媒活性比較………………62
5-3 操作參數之探討…………………………………65
5-3-1 不同NO進流濃度對NO轉化率之影響………65
5-3-2 空間速度的大小對NO轉化率之影響………67
5-3-3 水氣濃度對NO轉化率之影響………………67
5-4 反應動力之推求…………………………………69

第六章、 結論……………………………………………77

參考文獻……………………………………………………79

附錄I R.H.與A.H.於室溫下之換算表…………………83

附錄II 實驗操作條件與原始數據………………………84

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