博碩士論文 102326022 詳細資訊




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姓名 陳岱羚(Dai-Ling Chen)  查詢紙本館藏   畢業系所 環境工程研究所
論文名稱 結合鈣鈦礦型觸媒及非熱電漿技術去除氣流中酚之研究
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摘要(中) 揮發性有機化合物之排放已受到公眾越來越多的關注,因為揮發性有機化合物之排放對人體與環境會造成不利的危害,其中酚是重要的揮發性有機化合物,它在低濃度是具有毒性的,透過吸入、攝取及眼睛或皮膚的接觸都會對人類健康造成不良的影響,此外,酚也是重要的臭味物質,因此如何有效控制其排放實刻不容緩。本研究以perovskite型觸媒結合非熱電漿技術去除氣流中揮發性有機物,藉由上述之實驗來探討電漿與催化反應間之加成效應。本研究分為兩個部份進行討論,第一部份以檸檬酸溶膠凝膠法合成perovskite型觸媒LaMnO3,藉Sr及Cu的添加來製備改質之LaMnO3觸媒,並比較LaMnO3、La0.8Sr0.2MnO3及La0.8Sr0.2Mn0.8Cu0.2O3三種觸媒之催化活性及基本特性探討。研究結果顯示La0.8Sr0.2Mn0.8Cu0.2O3於200oC即可達到100%之去除效率且在300oC對酚之礦化率已達100%,而La0.8Sr0.2MnO3及LaMnO3則需於300oC及400oC才可達完全去除之效率。從觸媒之測試結果顯示改質之La0.8Sr0.2Mn0.8Cu0.2O3對酚之去除具有最佳活性。第二部份以非熱電漿及電漿觸媒系統去除酚,結果顯示在電壓為16 kV、頻率為8 kHz及總流率為300 mL/min之條件下,非熱電漿系統對於酚之去除率為80%,填充La0.8Sr0.2Mn0.8Cu0.2O3觸媒於非熱電漿系統中酚之去除效率達100%;礦化率則從11%上至55%提升了44%;能量效率方面,單階段電漿結合觸媒系統顯著高於單獨非熱電漿系統。整體而言,單階段電漿結合觸媒系統是有效提升非熱電漿處理氣流中酚之能量效率以及礦化率。
摘要(英) Emission of volatile organic compounds (VOCs) into atmosphere has received increasing public concern due to their adverse effects on human health and the environment. Phenol (C6H5OH) is one of the most important VOCs. It is toxic even at a low concentration, causing adverse effect on human health through inhalation, ingestion, or eye and skin contact. Additionally, it is also an important odor-causing substance and how to effectively control its emission remains a big challenge. This study aims to combine perovskite catalyst and non-thermal plasma in removing phenol from gas streams. Moreover, possible synergism caused by catalysis and plasma for VOCs removal is also investigated. The study is divided into two parts for discussion, the first part is the preparation of perovskite-type catalyst by citric acid method. LaMnO3 catalyst is substituted by Sr and Cu elements, and the catalytic activity and fundamental characteristics of the three catalysts including LaMnO3, La0.8Sr0.2MnO3 and La0.8Sr0.2Mn0.8Cu0.2O3 are compared. The results show that phenol removal efficiency achieved with La0.8Sr0.2Mn0.8Cu0.2O3 is up to 100% at the operating temperature of 200oC and the mineralization rate at 300oC is up to 100%, while the phenol removal efficiencies achieved with La0.8Sr0.2MnO3 and LaMnO3 are up to 100% at the operating temperature of 300oC and 400oC, respectively. The results show that La0.8Sr0.2Mn0.8Cu0.2O3 has the best activity of removal of phenol. Non-thermal plasma and combined plasma catalysis (CPC) are also applied to remove phenol from gas streams. The results show that with the condition of applied voltage of 16 kV, frequency of 8 kHz and flow rate of 300 mL/min, the phenol removal efficiency achieved with non-thermal plasma is 80%, and the phenol removal efficiency achieved with the combined plasma catalysis by filling La0.8Sr0.2Mn0.8Cu0.2O3 is up to 100%. Mineralization rate is improved by 44% as CPC is applied. For energy efficiency, the single-stage plasma catalysis is better than non-thermal plasma alone. Overall, the combined plasma catalysis is effective in enhancing the energy efficiency and mineralization rate of removing phenol from gas streams.
關鍵字(中) ★ 揮發性有機物
★ 酚
★ 非熱電漿技術
★ Perovskite型觸媒
★ 單階段電漿結合觸媒系統
關鍵字(英) ★ Volatile Organic Compounds
★ Phenol
★ Non-thermal plasma
★ Perovskite-type catalyst
★ Single-stage plasma catalysis
論文目次 摘要 I

Abstract II

目錄 III

圖目錄 VI

表目錄 IX

第一章 前言 1

1.1研究緣起 1

1.2研究目的 2

第二章 文獻回顧 3

2.1揮發性有機物之簡介 3

2.1.1揮發性有機物之定義及來源 3

2.1.2揮發性有機物之危害及來影響 4

2.1.3國內VOCs排放管制法規 8

2.1.4揮發性有機物之傳統控制技術 9

2.2實驗選定進行研究之揮發性有機物特性 11

2.3電漿 15

2.3.1電漿之生成原理 15

2.3.2電漿種類 16

2.4電漿去除VOCs之反應機制 21

2.5 Perovskite型觸媒 24

2.5.1 Perovskite型觸媒介紹 24

2.5.2 Perovskite型觸媒應用於VOCs之去除 25

2.6電漿觸媒系統 29

2.6.1單階段式電漿結合觸媒之機制 30

第三章 研究方法 38

3.1研究流程及架構 38

3.2預備實驗 40

3.2.1觸媒材料製備 40

3.2.2觸媒材料之物化特性分析 41

3.3實驗分析方法 44

3.3.1酚之分析方法及檢量線製作 44

3.4實驗系統 45

3.4.1實驗藥品與氣體 48

3.4.2連續進流的VOCs產生系統配置 49

3.4.3 VOCs去除測試系統配置 51

3.4.4採樣及分析系統 51

3.5研究方法 54

3.5.1觸媒活性反應實驗 54

3.5.2電漿觸媒反應實驗 55

3.6實驗結果之計算 56

第四章 結果與討論 58

4.1 觸媒之基本特性分析結果 58

4.1.1 BET氮氣吸脫附測試 58

4.1.2 SEM-EDS觸媒元素組成 59

4.1.3 XRD晶相分析 59

4.1.4 FE-SEM分析 60

4.1.5 ESCA特性分析 62

4.2 Perovskite型觸媒之活性測試 66

4.2.1溫度對酚去除之影響 66

4.2.2空間流速對酚去除之影響 67

4.2.3穩定性測試 68

4.2.4反應動力探討 69

4.2.5副產物生成探討 72

4.3單階段電漿結合觸媒對去除酚之影響 73

4.3.1 輸入電壓對酚去除之影響 73

4.3.2 輸入頻率對酚去除之影響 78

4.3.3不同載氣對酚去除之影響 79

4.3.4濕度對酚去除之影響 81

4.3.5進流酚濃度對去除效率之影響 83

4.3.6氣體停留時間對酚去除之影響 84

4.4 最終產物分析 85

4.4.1空氣下操作 85

4.4.2 添加不同Ar含量下操作 89

4.5 SPC去除酚之交互作用及反應途經推估 91

4.5.1 酚反應途徑推估 91

第五章 結論與建議 94

5.1 結論 94

5.2建議 95

參考文獻 96

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指導教授 張木彬(Moo-Been Chang) 審核日期 2015-8-25
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