臺灣博碩士論文加值系統

選擇性觸媒還原法(Selective Catalytic Reduction, SCR)是目前處理燃燒後廢氣中氮氧化物最有效的方法。本研究探討常用之V / Ti觸媒負載於(1)陶瓷纖維載體、(2)菫青石蜂巢以及(3)勃姆石沸石等三種載體，以評估不同載體對於V / Ti觸媒脫硝效率之影響。於本研究中發現將V15 / Ti85比例的觸媒以含浸法負載於陶瓷纖維載體後，在模擬煙道氣環境中空間速度3000 hr-1、氧氣濃度10 vol %、NO濃度450 ppm、NH3濃度500 ppm以及水氣濃度10 vol %下，在反應溫度250 oC時，NO轉化效率可達到96.3 %，並且N2O的產生量為12.8 ppm；同時在相同模擬條件下的煙道氣環境中，菫青石蜂巢的NO轉化效率為91.7 %，N2O的產生量為8.5 ppm；勃姆石沸石的NO轉化效率為23.1 %，N2O的產生量為9.0 ppm。於拉曼光譜分析結果得知，陶瓷纖維濾材與菫青石蜂巢這二種載體在含浸了V / Ti觸媒後，在拉曼光譜下的405、480與527 cm-1處的波峰有發現V-O和V-O-V的彎曲模式，由此可見增加釩氧化物在表面的分布有助於提高觸媒的脫硝效果。將觸媒漿液含浸到載體時，陶瓷纖維載體僅需含浸一次即可負載0.6 g的觸媒於載體上，菫青石蜂巢需含浸二次，勃姆石沸石需含浸三次。綜合以上結果，陶瓷纖維作為載體時，負載觸媒過程較為簡易，製作成本較低，此外負載在陶瓷纖維載體的脫硝觸媒，其NO轉化效率優於商用化許久的菫青石蜂巢載體。

Selective Catalytic Reduction is currently the most effective technique for removal of nitrogen oxides from post-combustion gases. In this study, three commonly used types of supports which loaded by V / Ti were investigated: (1) ceramic fiber, (2) cordierite honeycomb and (3) boehmite zeolite, in order to evaluate the effect of various supports loaded by V / Ti catalyst on the removal efficiency. In this work, the ratio of V15 / Ti85 was dispersed on the ceramic fiber through impregnation method, the conversion efficiency of NOx reached 96.3 % at the reaction temperature of 250 oC under the condition of space velocity was 3000 hr-1, the oxygen concentration was 10 vol %, the NO and NH3 concentration was 450 ppm and 500 ppm, respectively, and 10 vol % of water content, moreover, the N2O concentration was only 12.8 ppm. Besides, the NO conversion efficiency of V15 / Ti85 was loaded on honeycomb and boehmite zeolite was 91.7 % and 23.1 %, respectively, and the N2O concentration was 8.5 ppm and 9.0 ppm, respectively. According to the spectrum of Raman, it can be observed that the V-O and V-O-V stretching peak at 405, 480 and 527 cm-1, after impregnating with V / Ti catalysts, therefore, increasing the distribution of vanadium oxide is benefit to enhance the NO removal efficiency. While above supports were impregnated into catalyst slurry, just soaking once then obtained that 0.6g V / Ti was loaded on the ceramic fiber, however, in order to disperse the same amount of V / Ti, the honeycomb required impregnated twice, and the boehmite zeolite even required impregnated three times. Based on these results, The ceramic fiber as a support is easy to disperse, and the production cost is rather low. Additionally, V / Ti catalyst were dispersed on the ceramic fiber has excellent de-NOx efficiency which better than commercial honeycomb.

摘 要 i
Abstract ii
誌謝 iv
目錄 v
表目錄 viii
圖目錄 ix
第一章、前言 1
1.1 研究起源 1
1.2 研究目的 2
第二章、文獻回顧 4
2.1 NOx危害與生成機制 4
2.1.1 NOx對環境與人體所造成的危害 4
2.1.2 NOx來源與生成機制 4
2.1.3 NOx控制技術種類與特點 7
2.2 選擇性觸媒還原(SCR)技術 7
2.2.1 SCR原理介紹 7
2.2.2 SCR進行機制 8
2.2.3 SCR觸媒種類 9
2.2.4 觸媒的製作方法 10
2.3 SCR觸媒載體 10
2.3.1 SCR觸媒載體種類 10
2.3.2 不同SCR觸媒載體所應用之系統配置 12
2.4 影響SCR反應效率之因素 14
2.4.1 SCR觸媒自身之特性 14
2.4.2 SCR觸媒反應環境之特性 16
第三章 研究方法與實驗步驟 24
3.1 研究方法與流程架構 24
3.2 實驗藥品與實驗設備 26
3.2.1 實驗藥品與材料 26
3.2.2 實驗氣體 26
3.2.3 觸媒檢測儀器 27
3.3 實驗樣品製作 28
3.3.1 SCR觸媒液樣品製作 28
3.3.2觸媒載體前處理 29
3.3.3 浸漬SCR觸媒到觸媒載體 29
3.4 實驗樣品之鑑定 29
3.4.1 NO / N2O分析 29
3.4.2 X射線繞射儀 33
3.4.3 掃描式電子顯微鏡 34
3.4.4比表面積分析 35
3.4.5 拉曼光譜分析 38
第四章 結果與討論 40
4.1 V / Ti觸媒與其含浸載體後脫硝試驗結果 40
4.1.1 不同V / Ti比例觸媒粉在不同流速下的脫硝效率以及N2O產生量 40
4.1.2 不同V / Ti比例觸媒含浸陶瓷纖維載體後，在不同流速下的脫硝效率以及N2O產生量 42
4.1.3 不同V / Ti比例觸媒含浸蜂巢載體後，在不同流速下的脫硝效率以及N2O產生量 44
4.1.4 不同V / Ti比例觸媒含浸沸石載體後，在不同流速下的脫硝效率以及N2O產生量 46
4.1.5 V15 / Ti85比例觸媒含浸不同載體後，在不同流速下的脫硝效率以及N2O產生量 48
4.1.6 V / Ti觸媒與其含浸載體後脫硝試驗小結 49
4.2 V / Ti觸媒與觸媒載體基本特性分析結果 49
4.2.1 SEM與mapping結果討論 49
4.2.2 XRD結果討論 52
4.2.3 BET結果討論 59
4.2.4 Raman結果討論 69
4.2.5 V / Ti觸媒與觸媒載體基本特性分析小結 72
第五章 結論 75
參考文獻 78

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