臺灣博碩士論文加值系統

本研究以活性碳吸附程序結合臭氧氧化針對甲基乙基酮蒸汽(MEK)進行研究。並探討吸附/氧化程序下，臭氧對活性碳上的MEK蒸汽影響及反應動力常數計算。
實驗結果顯示隨著實驗條件不同，1000 ppmv臭氧對MEK蒸汽的破壞效率在12.4%到48.5%間。以Power law 動力模式計算出此反應的動力常數k’為0.0438 h-1，配合Arrhenius 方程式得到A為189.54h-1及Ea為5.12Kcal/mole。另以Langmuir-Hishelwood模式(Escobar et al., 2004)得到動力參數 為0.035及 為0.6183。最後，以modified Wheeler方程式(Wood and Moyer, 1989; Yoon and Nelson, 1984; Busmundrud, 1993)結合Power law動力或Langmuir-Hishelwood方程式能有效地預測此吸附/氧化反應之貫穿曲線。MEK蒸汽的破壞效率會隨著活性碳床及臭氧濃度的增加而提升。
本研究也利用有機金屬-化學氣相沉積法製備含有觸媒特性之活性碳進行吸附/氧化MEK實驗。並利用BET, ICP/AES及SEM/EDX等製備去分析Cu/AC之物化特性。此外，亦進行熱脫附實驗以求出其脫附動力參數E, A, 及n。其算出的最佳參數為熱脫附反應級數n=1.5且R-square值大於0.88。AC/O3之熱脫附能為22.67至18.32 kJ/mole (303–363 K)而Cu/AC/O3之熱脫附能為29.32至10.64 kJ/mole (303–363 K)。
當臭氧濃度增加到7800 ppmv且活性碳床重重加至5克，即使在長時間操作下MEK蒸汽的破壞效率亦會大於95﹪。未來吸附程序結合臭氧氧化對VOCs及臭味空氣污染控制有極大潛力。

This study attempts to combine the technologies of adsorption of volatile organic compound (VOC) on activated carbon and oxidation of VOC by O3. In the adsorption/oxidation process, the effects of ozone for the adsorption characteristics of methyl ethyl ketone (MEK) vapor on activated carbon are investigated. The kinetic parameters of reaction for MEK vapor and O3 on activated carbon are also determined. The results show that the destructive efficiencies of MEK by 1000 ppmv O3 on activated carbon are from 12.4 % to 48.5 %. From the power law kinetic model, the apparent kinetic constant, k, is obtained having a value of 0.0438 h-1 in this process. Moreover, the activation energy, Ea, is found to be 5.12 Kcal/mole and the value of rate constant, A, is 189.54 h from the analytical results of the Arrhenius equation. The Langmuir-Hishelwood model (Escobar et al., 2004) is also used to determined the kinetics parameters of and . The values are found to be 0.035 and 0.6183, respectively. Finally, the modified Wheeler equation (Wood and Moyer, 1989; Yoon and Nelson, 1984; Busmundrud, 1993) in combination with the power law kinetic model or Langmuir-Hishelwood is used to predict the breakthrough curves. The destruction of MEK can be effectively promoted as the bed height of activate carbon and the concentration of ozone increase.
The pretreatment of the metal-organic chemical vapor deposition process is used to modify the characteristics of the activated carbon The pore and surface characteristics of various adsorbents are analyzed by BET, ICP/AES, and SEM/EDX. In addition to this, desorption experiments are performed in a thermogravimetric analyzer. The kinetics parameters, E, A, and n, of thermal desorption from spent adsorbents saturated with MEK vapor are also calculated. The kinetic parameters, E, A, and n, of thermal desorption from the spent adsorbents saturated with MEK vapor are calculated according to the differential method. The optimum fitting results are where n=1.5. The differential method has a better fitting curve and all the fitting R-square values are more effective than 0.88. The apparent activation energy of AC with 1000 ppmv O3 for MEK vapor are 22.67 – 18.32 kJ/mole (303–363 K)and the apparent activation energy of Cu/AC with 1000 ppmv O3 for MEK vapor is 29.32- 10.64 kJ/mole(303 -363K).
The destructive efficiency of MEK is still greater than 95% even after a prolonged operational time when ozone concentration is increased to 7800 ppmv and the amount of activated carbon is increased to 5 g. From the results of this study, adsorption process in combination with ozone oxidation shows potential for the control of VOCs and odor.

第一章 緒論……………………………………………………………….. 1
1.1 前言…………..………………………………………………………1
1.2 研究背景……..………………………………………………………2
1.3 研究目的……..………………………………………………………4
1.4 研究內容……..………………………………………………………5
第二章 文獻回顧…….…………….………………………………………… ..…..6
2.1 VOCs相關文獻…………………………………………………………6
2.2 活性碳吸附VOCs相關文獻….…………………………………………10
2.3 觸媒氧化VOCs相關文獻…….………………………………………...30
2.4 臭氧氧化VOCs相關文獻…….………………………………………...42
2.5 活性碳吸附/觸媒氧化VOCs反應動力文獻….………………………..46
第三章 研究方法…………….………………………………………………..…..51
3.1研究流程…..……………….…………………………………………...51
3.2反應物製備……………………………………………………………...55
3.3 Cu/AC之物化特性分析方法…………………………………………......58
3.4 VOC選用…………………….……………………………………………63
3.5等溫吸附MEK蒸汽實驗….………………………………………………...64
3.6吸附/氧化MEK蒸汽實驗…………………………………………………...66
3.7熱脫附分析...…………………………………………………………….......69
第四章 結果與討論…………………………………………………..…………..71
4.1 空床實驗………………......… ………………………………………...71
4.2 活性碳吸附MEK蒸汽………………………………………………...73
4.3臭氧對活性碳吸附/氧化MEK蒸汽之影響………………………80
4.4 活性碳床動力模式………………………………………………..........90
4.5 活性碳床之MEK蒸汽吸附氧化貫穿曲線預測………………………...97
4.6 Cu/AC物化特性…………………………………………………………104
4.7 Cu/AC與AC吸附/氧化MEK蒸汽比較………………………………112
4.8 臭氧濃度對MEK蒸汽吸附氧化影響………………………………….132
4.9 AC與Cu/AC熱脫附比較……………………………………………….134
第五章 結論與建議………..……………………………………………..…146
5.1 結論……………….....…………………………………………………..146
5.2 建議……………….....…………………………………………………..147
參考文獻




















圖 目 錄

圖2-1. VOCs處理之相對費用 9
圖2-2. 吸附劑之孔洞大小分佈比較 11
圖2-3. 活性碳表面酸性基團 20
圖2-4. 活性碳床吸附VOC示意圖 27
圖2-5. MEK熱分解之反應機構 40
圖3-1. 研究流程 53
圖3-2. 吸附/氧化實驗裝置 54
圖3-3. MO-CVD裝置 57
圖3-4. BET總表面積極孔隙測定儀 59
圖3-5. ICP/AES分析銅離子標準濃度檢量線 62
圖4-1. 臭氧對MEK蒸汽濃度影響 72
圖4-2. 1 g AC在不同MEK蒸汽進口濃度之貫穿曲線(303K) 74
圖4-3. 1 g AC在不同MEK蒸汽進口濃度之貫穿曲線(323K) 74
圖4-4. 1 g AC在不同MEK蒸汽進口濃度之貫穿曲線(343K) 75
圖4-5. 1 g AC在不同MEK蒸汽進口濃度之貫穿曲線(363K) 75
圖4-6. 1 g AC在不同溫度下100 ppmv MEK蒸汽貫穿曲線 76
圖4-7. 1 g AC 在不同溫度下300 ppmv MEK蒸汽貫穿曲線 76
圖4-8. 1 g AC在不同溫度下1000 ppmv MEK蒸汽貫穿曲線 77
圖4-9. 不同溫度下MEK蒸汽之等溫吸附曲線 79
圖4-10.不同活性碳床高對MEK蒸汽之破壞效果
(100 ppmv MEK蒸汽、1000 ppmv O3、303 K) 82
圖4-11. MEK蒸汽吸附氧化操作時間對濃度分率微分圖
(100 ppmv MEK蒸汽、1000 ppmvO3、303 K) 82
圖4-12. MEK蒸汽吸附/氧化程序之吸附量計算方法 83
圖4-13. MEK蒸汽停留時間對破壞效果關係
(100 ppmv MEK、1000ppmv O3、303 K) 84
圖4-14.反應溫度對MEK蒸汽之吸附氧化效果影響
(300 ppmv MEK、1000 ppmv O3、1 g AC) 87
圖4-15.反應溫度對MEK蒸汽之吸附氧化效果影響
(1000 ppmv MEK、1000 ppmv O3、1 g AC) 87
圖4-16. MEK蒸汽吸附氧化操作時間對濃度分率微分圖
(300 ppmv MEK蒸汽、1000 ppmvO3、303 K) 88
圖4-17. MEK蒸汽吸附氧化操作時間對濃度分率微分圖
(1000 ppmv MEK蒸汽、1000 ppmvO3、303 K) 88
圖4-18. Power Law 動力模式預測
(100 ppmv MEK vapor、1000 ppmv O3、303 K) 91
圖4-19. 1000 ppmv O3之Power Law動力模式預測 93
圖4-20. Langmuir-Hinshelwood動力模式預測
(100 ppmv MEK vapor、1000 ppmv O3、303 K) 96
圖4-21. Modified Wheeler equation貫穿曲線模式預測
(100 ppmv MEK vapor、1000 ppmv O3、303 K) 98
圖4-22. Modified Wheeler equation貫穿曲線模式預測
(300 ppmv MEK vapor、1000 ppmv O3、1 g AC) 98
圖4-23. Modified Wheeler equation貫穿曲線模式預測
(1000 ppmv MEK vapor、1000 ppmvO3、5 g AC) 99
圖4-24. Power law模式配合Modified Wheeler貫穿曲線模式預測
(100 ppmv MEK vapor、1000 ppmvO3、303 K) 100
圖4-25. Power law模式配合Modified Wheeler貫穿曲線模式預測
(300 ppmv MEK vapor、1000 ppmv O3、1 g AC) 100
圖4-26. Power law模式配合Modified Wheeler貫穿曲線模式預測
(1000 ppmv MEK vapor、1000 ppmv O3、5 g AC) 101
圖4-27. L-H模式配合Modified Wheeler貫穿曲線模式預測
(100 ppmv MEK vapor、1000 ppmv O3、303 K) 102
圖4-28. MO-CVD操作溫度對Cu/AC的影響 105
圖4-29. MO-CVD反應時間對Cu/AC的影響 105
圖4-30. EDS patterns of Cu/AC by MO-CVD process 108
圖4-31. XRD patterns of AC and Cu/AC by MO-CVD process 109
圖4-32. AC之SEM圖(比例尺300 μm) 110
圖4-33. AC之SEM圖(比例尺10 μm) 110
圖4-34. AC之SEM圖(比例尺6 μm) 110
圖4-35.樣品1之Cu/AC之SEM圖(比例尺300 μm) 111
圖4-36.樣品2之Cu/AC之SEM圖(比例尺300 μm) 111
圖4-37.樣品3之Cu/AC之SEM圖(比例尺300 μm) 111
圖4-38.樣品3之Cu/AC之SEM圖(比例尺6 μm) 111
圖4-39. Cu/AC與AC吸附300 ppmv MEK蒸汽貫穿曲線比較 113
圖4-40. Cu/AC與AC吸附1000 ppmv MEK蒸汽貫穿曲線比較 113
圖4-41. Cu/AC與AC吸附氧化300 ppmv MEK蒸汽貫穿曲線比較 117
圖4-42. Cu/AC與AC吸附氧化1000 ppmv MEK蒸汽貫穿曲線比較 117
圖4-43. MEK蒸汽吸附氧化之操作時間對濃度分率微分圖
(300 ppmv MEK蒸汽、1000 ppmv O3、1 g Cu/AC) 118
圖4-44. MEK蒸汽吸附氧化之操作時間對濃度分率微分圖
(1000 ppmv MEK蒸汽、1000 ppmv O3、5 g Cu/AC) 118
圖4-45. 1000 ppmv O3吸附氧化300 ppmv MEK蒸汽之Power law 動力模式預測 121
圖4-46. 1000 ppmv O3吸附氧化1000 ppmv MEK蒸汽之Power law 動力模式預測 121
圖4-47. Langmuir-Hinshelwood動力模式預測(300ppmv MEKvapor、1000ppmv O3) 124
圖4-48. Langmuir-Hinshelwood動力模式預測(1000ppmv MEKvapor、1000ppmv O3) 124
圖4-49. 300 ppmv MEK及1 g Cu/AC之power law模式預測φ值配合Modified Wheeler貫穿曲線模式預測 129
圖4-50. 1000 ppmv MEK及5 g Cu/AC之power law模式預測φ值配合Modified Wheeler貫穿曲線模式預測 129
圖4-51. 300 ppmv MEK及1 g AC之L-H模式預測φ值配合Modified Wheeler貫穿曲線模式預測 130
圖4-52. 1000 ppmv MEK及5 g AC之L-H模式預測φ值配合Modified Wheeler貫穿曲線模式預測 130
圖4-53. 300 ppmv MEK及1 g Cu/AC之L-H模式預測φ值配合Modified Wheeler貫穿曲線模式預測 131
圖4-54. 1000 ppmv MEK及5 g Cu/AC之L-H模式預測φ值配合Modified Wheeler貫穿曲線模式預測 131
圖4-55. 2000 ppmv MEK蒸汽在不同濃度臭氧的貫穿曲線(303 K) 133
圖4-56. AC和Cu/AC利用TGA脫附MEK之TGA比較圖(303K) 139
圖4-57. AC和Cu/AC利用TGA脫附MEK之DTA比較圖(303K) 139
圖4-58. AC和Cu/AC利用TGA脫附MEK之TGA比較圖(343K) 140
圖4-59. AC和Cu/AC利用TGA脫附MEK之DTA比較圖(343K) 140
圖4-60. AC和Cu/AC配合臭氧反應後之TGA比較圖(303K) 141
圖4-61. AC和Cu/AC配合臭氧反應後之DTA比較圖(303K) 141
圖4-62. AC和Cu/AC配合臭氧反應後之TGA比較圖(323K) 142
圖4-63. AC和Cu/AC配合臭氧反應後之DTA比較圖(323K) 142
圖4-64. AC和Cu/AC配合臭氧反應後之TGA比較圖(343K) 143
圖4-65. AC和Cu/AC配合臭氧反應後之DTA比較圖(343K) 143
圖4-66. AC和Cu/AC配合臭氧反應後之TGA比較圖(363K) 144
圖4-67. AC和Cu/AC配合臭氧反應後之DTA比較圖(363K) 144


表 目 錄
表2-1. 常見之揮發性有機物處理技術 9
表2-2. 物理吸附及化學吸附比較 14
表2-3. 活性碳碳表面含氧官能基 22
表2-4. 觸媒氧化VOCs文獻整理 31
表2-5. MEK蒸汽氧化之反應機構 41
表2-6. 臭氧去除方法主要優點及缺點比較 44
表3-1. 活性碳基本性質 55
表3-2. ASAP 2000型孔隙分析儀設備規格 59
表3-3. MEK基本物化特性 63
表3-4. 重量法標定MEK蒸汽濃度 65
表3-5. GC/FID操作參數設定 65
表3-6. 研究設備及廠牌規格 68
表4-1. 活性碳吸附MEK蒸汽之吸附特性 77
表4-2. 活性碳吸附蒸汽之Langmuir飽和吸附量預測 79
表4-3. 床高對臭氧破壞100 ppmv MEK蒸汽影響(1000 ppmv O3、303 K) 84
表4-4. 反應溫度對AC配合1000 ppmv O3吸附氧化MEK蒸汽影響 89
表4-5. AC配合1000 ppmv O3吸附氧化MEK蒸汽之貫穿曲線預測 99
表4-6. Power law配合Modified Wheeler對AC吸附氧化MEK蒸汽貫穿曲線預測 101
表4-7. L-H配合Modified Wheeler對AC吸附氧化MEK蒸汽貫穿曲線預測 102
表4-8. AC吸附氧化MEK蒸汽之實驗φ值與動力預測之φ值比較 103
表4-9. The pore and surface characteristics of AC and Cu/AC 108
表4-10.Cu/AC與AC在不同吸附溫度之單成分MEK蒸汽吸附比較 114
表4-11.Cu/AC與AC之吸附氧化停留時間與剩餘因子比較 119
表4-12. AC吸附氧化MEK蒸汽之實驗φ值與動力預測之φ值比較 125
表4-13. 1000 ppmv O3吸附氧化MEK蒸汽貫穿曲線預測(Power law) 127
表4-14. 1000 ppmv O3吸附氧化MEK蒸汽貫穿曲線預測(L-H) 128
表4-15. AC與Cu/AC熱脫附動力數據 145

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U論文發表
博士論文
含銅活性碳吸附結合臭氧氧化程序處理揮發性有機氣體，指導教授尤建華，now。
碩士論文
以電化學薄膜程序處理低濃度含銅重金屬廢水，指導教授尤建華，2001。
學士論文
熱敏感乳液於固定酵素上之應用，指導教授陳志平，1999。
Paper
Wu, H.M., and J.H. You, "Adsorption of activated carbon in combination with ozone oxidation for odor control of diethyl-amine vapor", Journal of the Chinese Institute of Environmental Engineering, Vol. 15, No. 3(2005).
Jiann-Hwa You, Hon-Ei Lin, and Hung-Ming Wu , " Effects of Relative Humidity on the Adsorption Characteristics for Methyl-Ethyl-Ketone Vapor on the Activated carbon ",Journal of the Chinese Institute of Environmental Engineering, Vol. 15, No. 1, pp. 47-56(2005).
Referee Paper
Wu, H.M., J.H. You," Adsorption of Activated Carbon with Copper in Combination with Ozone Oxidation for MEK Vapor Control", The 5PthP World Congress on Oxidation Catalysis, Sapporo, Japan, September 25-30(2005).
尤建華、吳泓明、周明杰，活性碳結合臭氧對MEK有機溶劑蒸氣吸附氧化特性探討，第十七屆中華民國環境工程年會暨第二十二屆空氣污染控制技術研討會，2005。
尤建華、曾耀諄、吳泓明，活性碳對丙酮及DMF有機溶劑蒸氣吸附特性及模式預測探討，第十屆海峽兩岸環境保護學術研討會，台中，十月(2005)。
尤建華、許坤炎、吳泓明，臭氧氧化前處理EDTA-Cu廢水的可行性，2005清潔生產暨永續發展研討會，2005。
吳泓明、尤建華，有機金屬化學沈積法前處理活性碳及結合臭氧吸附氧化處理臭味控制研究，第十六屆中華民國環境工程年會暨第二十一屆空氣污染控制技術研討會，2004。
吳泓明、尤建華，高濃度臭氧結合含銅活性碳對MEK蒸汽吸附氧化之研究，中國化學工程學會九十三年年會暨國科會化學工程學門成果發表會，2004。
J.H. You, H. M. Wu and Z. X. Fang , "Surface Fractal Dimensions of adsorbent from industrial sludge", The Third Pacific Basin Conference on Adsorption Science and Technology, Kyongju, Korea, May 25-29 (2003).
吳泓明、尤建華，以電化學薄膜程序處理低濃度含銅重金屬廢水，中國化學工程學會九十二年年會國科會化學工程學門成果發表會，2003。
尤建華、林宏育、吳泓明，濕度對甲基乙基酮與甲苯有機蒸氣的吸附特性影響比較，第十四屆中華民國環境工程年會暨第十九屆空氣污染控制技術研討會，國科會研究計畫編號NSC89-2211-E-182-003，2002。
尤建華、陳逸傑、吳泓明、吳逢昌，焦磷酸重金屬廢水處理研究，台塑集團應用工程技術研討會，2001。