以臭氧催化氧化與電漿催化系統氧化一氧化氮之效率探討

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林昱衡(Yu-Heng Lin) 查詢紙本館藏

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論文名稱

以臭氧催化氧化與電漿催化系統氧化一氧化氮之效率探討

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摘要(中)

本研究致力於開發低溫高效之一氧化氮氧化技術，並比較電漿催化與臭氧催化氧化兩種控制技術，分別針對流量、反應溫度、氣流組成及觸媒穩定性進行測試，並探討各操作參數對NO氧化效率之影響。本研究使用兩種錳金屬前驅物浸漬於TiO2 (P25)以製備FeMn/TiO2觸媒，分別為硝酸錳與醋酸錳，並比較兩者對觸媒催化活性之影響。電漿催化系統之操作條件為270 ppm NO、氧含量20%、氣體流量1.2 L/min、空間速度15,000 h-1，結果顯示使用FeMn/TiO2 (MA)觸媒展現較佳之NO氧化效率，於SED =520 J/L時NO氧化效率達70±1.2%，然而氣流中含250 ppm SO2時，NO氧化效率下降至53±1.5%。使用臭氧機生成臭氧，於室溫下進行NO深度氧化，系統之操作條件為270 ppm NO、氣體流量2.5 L/min，O3/NO =1時，NO氧化效率達100%，生成212±5.0 ppm NO2，當O3/NO¬ =1.9時可將NO2完全氧化，生成97±3.1 ppm N2O5。臭氧催化氧化系統以FeMn/TiO2 (MA)為觸媒，溫度上升可促進N2O5生成，於反應溫度100℃、空間速度15,000 h-1，O3/NO =1.7時，N2O5濃度由60±4.9 ppm上升至101±5.6 ppm。觸媒之物化特性分析結果顯示FeMn/TiO2 (MA)觸媒具有較高之比表面積及孔體積，分別為47.4 m2/g及0.34 cm3/g，且此觸媒具有高比率之吸附氧(Oα)及Mn3+物種，可提升觸媒之催化活性，進而促進NO之氧化效率。

摘要(英)

This study aims to develop a low-temperature, and high-efficiency technology for the oxidation of nitrogen oxide (NOx). Moreover, comparison of the catalyst for plasma catalysis and ozone catalytic oxidation (OZCO) is conducted. FeMn/TiO2 catalysts were prepared through the impregnation of manganese acetate (MA) or manganese nitrate (MN) precursors on TiO2 (P25) and tested for the oxidation of NO. Experimental results indicate that FeMn/TiO2 (MA) catalyst shows higher activities for NO oxidation if compared with FeMn/TiO2 (MN) catalyst. As the inlet NO concentration is controlled at 270 ppm, the NO oxidation efficiency could achieve 70±1.2% at SED =520 J/L. However, existence of SO2 lower the efficiency of NO oxidation. The NO oxidation efficiency dropped to 53±1.5%. The deep oxidation of NO by ozone could achieve 100% efficiency at O3/NO =1 and room temperature, NO2 concentration is measured as 212±5.0 ppm. NO2 is almost completely oxidized at O3/NO =1.9, producing 97±3.1 ppm N2O5. The concentration of N2O5 increased to 101±5.6 ppm as the temperature was increased to 100℃ at O3/NO =1.7 by the OZCO method. Characterization of catalyst indicates that FeMn/TiO2 (MA) catalyst has a higher BET specific surface area and pore volume, which are 47.4 m2/g and 0.34 cm3/g, respectively. Moreover, this catalyst has good oxidation property to promote NO oxidation due to higher Oα/Oβ and Mn3+/Mn4+ ratio.

關鍵字(中)

★ 一氧化氮
★ 臭氧
★ 電漿催化
★ NO深度氧化
★ 臭氧催化氧化

關鍵字(英)

★ nitric oxide
★ ozone
★ plasma catalysis
★ NO deep oxidation
★ ozone catalytic oxidation

論文目次

摘要 I
目錄 III
圖目錄 VI
表目錄 VIII
第一章前言 1
1.1. 研究源起 1
1.2. 研究目的 3
第二章文獻回顧 4
2.1 氮氧化物之介紹 4
2.1.1 氮氧化物的特性與來源 4
2.1.2 氮氧化物之生成機制 5
2.2 氮氧化物之控制技術 6
2.3 非熱電漿技術原理 9
2.3.1 NTP污染物去除機制 9
2.3.2 NTP反應器的種類 11
2.4 NTP去除污染物之影響因素 15
2.4.1 NTP反應器結構 17
2.4.2 電源供應參數 17
2.4.3 氣流組成 19
2.5 NTP-觸媒整合系統 21
2.6 NTP-觸媒整合系統應用於臭氧生成 23
2.7 以臭氧氧化氮氧化物 26
2.8 臭氧氧化NO之影響因素 26
2.9 觸媒對NO深度氧化 29
第三章研究方法 32
3.1. 研究流程與架構 32
3.2. 觸媒選擇及製備 34
3.2.1. 觸媒材料選擇 34
3.2.2. 觸媒製備 34
3.3. 觸媒之物化特性分析 35
3.4. NO氧化實驗 37
3.4.1. 電漿催化系統 37
3.4.2. 臭氧催化氧化系統 39
3.4.3. 實驗分析 40
3.5. 動力學分析 42
3.6. 實驗結果之計算 43
3.7. 實驗之材料與設備 44
第四章結果與討論 47
4.1. 觸媒特性分析 47
4.1.1. X光粉末繞射儀(XRD)晶相鑑定 47
4.1.2. X射線光電子能譜儀(XPS)分析 48
4.1.3. 觸媒之物理特性分析 50
4.2. 電漿催化對NO氧化效率之探討 52
4.2.1. 電漿催化系統之NOx濃度變化 53
4.2.2. O2對NO氧化效率之影響 55
4.2.3. SO2對NO氧化效率之影響 56
4.3. DBD電漿產生臭氧進行NO深度氧化 57
4.4. 臭氧分解測試 61
4.5. 臭氧催化氧化NO之效率探討 63
4.5.1. 溫度對臭氧催化氧化NO之影響 66
4.5.2. 臭氧氧化NO之動力分析 68
第五章結論與建議 71
參考文獻 73

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指導教授

張木彬(Moo-Been Chang)

審核日期

2022-9-29

推文