以電漿觸媒系統去除氣流中CFC-12及HCFC-22之可行性探討

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溫馨(Shin Wen) 查詢紙本館藏

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論文名稱

以電漿觸媒系統去除氣流中CFC-12及HCFC-22之可行性探討
(Removal of CFC-12 and HCFC-22 from Gas Stream via Combined Plasma Catalysis)

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摘要(中)

工業及生活中常用的冷媒材料為含鹵素之化合物，如氟氯碳化合物(chlorofluorocarbons, CFCs)或含氫之氟氯碳化合物(hydrochlorofluorocarbons, HCFCs)。由於CFCs及HCFCs的化學穩定性，最終將由對流層擴散至平流層，並經由光解反應釋出氯原子進而破壞平流層臭氧，此外CFCs及HCFCs具高全球暖化潛勢(Global warming potential, GWP)對全球暖化亦有影響，現行處理CFCs及HCFCs相關技術包括高溫焚化、觸媒催化及電漿技術等。本研究旨在分析電漿觸媒系統對於氣流中CFC-12及HCFC-22之去除效率及機制，並可分成三個部分：(1)去除CFC-12及HCFC-22之電漿觸媒系統開發；(2)進行電漿觸媒之機制分析；(3) 評估其可行性與對環境之效益。結果顯示利用電漿觸媒法具有去除CFC及HCFC之可行性，在進流濃度為800 ppm、總流量為500 sccm、添加1%O2且操作電壓為17 kV時，CFC-12及HCFC-22之最高去除效率分別達99.0%及99.4%，其能量效率分別為4.9 g/kWh及3.3 g/kWh；CFC-12及HCFC-22經電漿反應後生成之副產物主要為CO2、NOX，此外因氮分子之解離能、電離電勢較激發為亞穩態分子N2(A3∑u+)高，加上CFC-12及HCFC-22具有較大的解離性電子反應截面易與高能電子反應，其去除機制主要經由電漿產生之N2(A3∑u+)及高能電子進行分解反應。

摘要(英)

Halogen-containing compounds including chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs) are widely used in industry. Due to their chemical stability, CFCs and HCFCs, gradually diffuse from the troposphere to the stratosphere and catalyze the destruction of ozone through photodegradation. In addition, high global warming potentials (GWP) of CFCs and HCFCs also aggravate global warming. Current technologies for treating CFCs and HCFCs include high-temperature incineration, catalysis, and plasma destruction. This study aims to develop a catalyst with good activity and combine it with a plasma reactor as a hybrid system for the removal of CFC-12 and HCFC-22. The study is divided into three parts: (1) Development of plasma catalyst system for removing CFC-12 and HCFC-22 (2) Elucidation of plasma catalysis mechanism (3) Assessment of feasibility and environmental benefit. The results show that combined plasma catalyst system is effective in removing CFC-12 and HCFC-22. The highest removal efficiencies of CFC-12 and HCFC-22 are 99.0% and 99.4% respectively as the operating conditions are controlled at applied voltage=17 kV, gas flow rate= 500 sccm, CFC-12 or HCFC-22= 800 ppm and O2= 1%. The byproducts produced by plasma reaction of CFC-12 and HCFC-22 are CO2, and NOX. The dissociation energy and ionization potential of nitrogen molecules are higher than that of excited metastable molecules (N2(A3∑u+)). In addition, CFC-12 and HCFC-22 are easy to react with high-energy electrons and have large dissociative electron reaction cross sections. Therefore, the main removal mechanism is the decomposition reaction of N2(A3∑u+) and high-energy electrons generated by plasma.

關鍵字(中)

★ 臭氧破壞物質
★ 電漿觸媒
★ CFC
★ HCFC
★ 全球暖化

關鍵字(英)

★ CFC
★ Global warming
★ Ozone depleting substances
★ Plasma catalysis
★ HCFC

論文目次

摘要 i
Abstract ii
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 4
2.1 CFCs及HCFCs 4
2.2 CFCs及HCFCs之去除技術 8
2.2.1 以觸媒催化去除CFCs及HCFCs 10
2.2.2 以電漿技術去除CFCs及HCFCs 14
2.3 DBD電漿結合觸媒進行CFCs或HCFCs之去除 25
第三章研究方法 31
3.1 研究方法 31
3.2 實驗設備、藥品與氣體 33
3.2.1 實驗設備 33
3.2.2 實驗藥品 36
3.2.3 實驗氣體 36
3.3 觸媒製備 37
3.4 CFC-12及HCFC-22去除實驗 38
3.4.1 熱催化實驗 38
3.4.2 電漿與電漿結合觸媒實驗 38
3.5 實驗之結果計算 41
3.6 觸媒特性分析 42
第四章結果與討論 45
4.1 觸媒熱催化對CFC-12去除效率之探討 45
4.1.1 不同觸媒對去除CFC-12之影響 45
4.1.2 氧氣含量之影響 46
4.2 觸媒熱催化對HCFC-22去除效率之探討 47
4.2.1 不同觸媒對於去除HCFC-22之影響 47
4.2.2 氧氣含量對HCFC-22去除效率之影響 48
4.3 DBD電漿反應對CFC-12去除效率之影響 50
4.3.1 不同觸媒對於CFC-12之影響 50
4.3.2 氧氣含量對CFC-12去除效率之影響 53
4.3.3 CFC-12進流濃度對去除效率之影響 55
4.3.4 氣體流量對CFC-12去除效率之影響 57
4.3.5 水氣對CFC-12去除效率之影響 59
4.3.6 能量效率 60
4.4 DBD電漿反應對HCFC-22去除效率之影響 64
4.4.1 不同觸媒對於HCFC-22之影響 64
4.4.2 氧氣含量對HCFC-22去除效率之影響 66
4.4.3 HCFC-22進流濃度對去除效率之影響 68
4.4.4 進流流量對HCFC-22去除效率影響 70
4.4.5 水氣對HCFC-22去除效率之影響 71
4.4.6 能量效率 73
4.5 產物分析 77
4.6 觸媒特性分析 89
4.6.1 BET氮氣吸脫附及SEM-EDS元素分析 89
第五章結論與建議 90
5.1 結論 90
5.2 建議 91
參考文獻 92

圖目錄
圖2- 1 CFC-11、CFC-12與CFC-113之歷年產量 6
圖2- 2常見之HCFC之歷年產量 7
圖2- 3歷年大氣環境中之CFC-12濃度趨勢 7
圖2- 4破壞臭氧層物質銷毀技術 9
圖2- 5以含鈀觸媒進行CFC-12加氫脫氯催化應機制 13
圖2- 6非熱電漿觸媒系統觸媒配置示意圖 28
圖3- 1研究流程 32
圖3- 2熱催化系統實驗設置 39
圖3- 3電漿觸媒系統實驗設置圖 40
圖4- 1溫度及添加不同觸媒對CFC-12去除效率之影響 45
圖4- 2氧氣含量對CFC-12去除效率之影響 46
圖4- 3 熱催化系統CFC-12去除效率隨反應時間之變化 47
圖4- 4溫度及添加不同觸媒對HCFC-22去除效率之影響 48
圖4- 5氧氣含量對HCFC-22去除效率之影響 49
圖4- 6 熱催化系統HCFC-22去除效率隨反應時間之變化 50
圖4- 7操作電壓及添加不同觸媒對CFC-12去除效率之影響 52
圖4- 8操作電壓及添加不同觸媒對CFC-12去除速率之影響 52
圖4- 9操作電壓及添加不同氧氣含量對CFC-12去除效率之影響 54
圖4- 10操作電壓及添加不同氧氣含量對CFC-12去除速率之影響 54
圖4- 11 電漿系統CFC-12去除效率隨反應時間之變化 55
圖4- 12含氧條件下CFC-12進流濃度及操作電壓對去除效率影響 56
圖4- 13含氧條件下CFC-12進流濃度及操作電壓對去除速率影響 57
圖4- 14進流流量及操作電壓對CFC-12去除效率之影響 58
圖4- 15進流流量及操作電壓對CFC-12去除速率之影響 58
圖4- 16水氣對CFC-12去除效率之影響 59
圖4- 17水氣對CFC-12去除速率之影響 60
圖4- 18填充不同觸媒對放電功率之影響 62
圖4- 19不同觸媒於不同操作電壓之能量效率 62
圖4- 20操作電壓及添加不同觸媒對HCFC-22去除效率之影響 65
圖4- 21不同操作電壓及觸媒對HCFC-22去除速率之影響 65
圖4- 22操作電壓及不同氧氣含量對HCFC-22去除效率之影響 67
圖4- 23操作電壓及不同氧氣含量對HCFC-22去除速率之影響 67
圖4- 24 電漿系統HCFC-22去除效率隨反應時間之變化 68
圖4- 25進流濃度及操作電壓對HCFC-22去除效率之影響 69
圖4- 26進流濃度及操作電壓對HCFC-22去除速率之影響 69
圖4- 27進流流量及操作電壓對HCFC-22去除效率之影響 70
圖4- 28進流流量及操作電壓對HCFC-22去除速率之影響 71
圖4- 29水氣對HCFC-22去除效率之影響 72
圖4- 30水氣對HCFC-22去除速率之影響 72
圖4- 31填充不同觸媒對放電功率之影響 74
圖4- 32填充不同觸媒於不同操作電壓之能量效率 75
圖4- 33放電前之CFC-12 FTIR圖譜 77
圖4- 34放電過程之CFC-12副產物FTIR圖譜 78
圖4- 35放電前之HCFC-22 FTIR圖譜 78
圖4- 36放電過程HCFC-22副產物之FTIR圖譜 79
圖4- 37 去除CFC-12於不同電壓下CO2產生之濃度 85
圖4- 38去除CFC-12於不同電壓下NO2產生之濃度 85
圖4- 39去除CFC-12於不同電壓下N2O產生之濃度 86
圖4- 40 HCFC-22於不同電壓產生之CO2含量變化 86
圖4- 41 HCFC-22於不同電壓產生之NO2含量變化 87
圖4- 42 HCFC-22於不同電壓產生之N2O含量變化 87
圖4- 43 CFC-12及HCFC-22於氮氣電漿且含氧氣氣流之反應途徑 88

表目錄
表2-1 CFC-12及HCFC-22之生命週期、GWP與ODP值 8
表2- 2 Oxidation &Hydrolysis —去除CFCs及HCFCs文獻彙整 16
表2- 3 Hydrodehalogenation去除CFC-12之相關文獻彙整 17
表2- 4 Hydrodehalogenation去除HCFC-22之文獻彙整 18
表2- 5熱電漿及非熱電漿基本性質 19
表2- 6非熱電漿技術去除CFC及HCFC之相關文獻 26
表2- 7非熱電漿技術去除CFC及HCFC之相關文獻 27
表3- 1 本研究所使用之藥品種類、濃度規格與供應廠商 36
表3- 2本研究使用之氣體種類及用途 36
表3- 3熱催化實驗操作參數 39
表3- 4電漿及電漿觸媒實驗操作參數 40
表4- 1非熱電漿系統去除CFC-12文獻比較 63
表4- 2非熱電漿系統去除HCFC-22文獻比較 76
表4- 3 CFC-12及HCFC-22於電漿中之反應及速率常數 82
表4- 4 Mn/TiO2 觸媒表面之元素組成與比表面積 89

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指導教授

張木彬(Moo-Been Chang)

審核日期

2020-8-24

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