過去研究針對染整廢水常以AOPs(Advanced Oxidation Processes , AOPs)程序中之Fenton法處理，然而Fenton法卻有污泥之後續處理問題。本研究以強氧化劑過硫酸鈉(Sodium persulfate, Na2S2O8)配合一般染整業排放廢水皆較高溫的特質，並結合UV光照射催化產生硫酸根自由基來降解染整業廢水色度。期待了解過硫酸鈉於不同溫度及配合UV光照射之染料去除效果與其限制，以及染料orange II降解之反應機制，如反應動力常數、半衰期、活化能等。
    實驗設計為過硫酸鈉分別在溫度20、40及60℃熱催化並結合UV光照射降解染料，以及在 NaPS/Dye = 15、7.5及1.5下，探討過硫酸鈉對偶氮染料orange II色度之去除狀況及氧化劑之使用量。
Orange II染料降解在本實驗條件中為擬一階動力反應，Orange II染料僅經由熱能並無法將其降解，當加入熱催化後過硫酸鈉鹽方可對色度行降解。且染料降解效率亦隨溫度上升而增加；此外，氧化劑量的增加(NaPS/Dye莫耳比增加)對染料降解效率亦可提昇，而降解速度也隨溫度提昇及NaPS/Dye莫耳比增加而增加。在60℃及NaPS/Dye =15條件下，有UV活化能為77.38KJ/mole，而無UV光照射下120.84 KJ/mole。
    相較於使用Fenton方法，本實驗方法實可以減少二次汙染問題，而再結合UV光照射輔助降解染料證實UV可以降低活化能而有效增加色度降解。

The past researchers investigating dyeing wastewater focused mainly on Fenton which is one of Advanced Oxidation Processes (AOPs). However, Fenton has the problem of generating large quantity of waste sludge. Taking the advantage of higher temperature in dyeing wastewater, in this study sodium persulfate (Na2S2O8) was thermally activated with or without UV radiation to produce sulfate radical for decolorization of dyeing wastewater. The aim of this work is to investigate the effects of temperature and Na2S2O8 dosges on decolorization of dye by thermally activated Na2S2O8 with or without UV radiation. Reaction kinetic parameters of dye orange II decolorization process such as pseudo-first-order reaction rate constant, half-life and activation energy are calculated.
    The decolorization of orange II azo dye with thermal activation of Na2S2O8with or without UV radiation are investigated at temperature of 20oC, 40oC, and 60oCand NaPS/Dye molar ratio of 15, 7.5, and 1.5. The decolorization of orange II follows the pseudo-first-order reaction rate kinetic. Increased Na2S2O8 dosges and temperature enhance the efficiency of decolorization. Under the condition of NaPS/Dye =15, the activation energy with UV radiation is 77.38KJ/mole; in the meanwhile, the activation energy without UV radiation is 120.84 KJ/mole.
    In contrast to Fenton, thermally activated Na2S2O8 can alleviate the problems of generating secondary waste sludge. Furthermore, the concepts that UV could decrease activation energy and increase the effectiveness of decolorization are supported by experimental results.

目錄	I
List of Figure	VI
List of Table	X
第一章 前言	1
1.1研究緣起	1
1.2研究目的	3
第二章 文獻回顧	4
2.1染料簡介	4
2.2染料顏色成因	4
2.3偶氮染料	5
2.4染整廢水之處理技術	7
2.4.1物理法	7
2.4.2化學法	7
2.4.3生物處理法	7
2.4.4高級氧化處理法	8
2.5過硫酸鹽介紹	9
2.5.1過硫酸鹽的沿用	9
2.5.2過硫酸鹽的特性	9
2.5.3過硫酸鹽自行分解反應	11
2.6常見氧化劑氧化還原電位比較	11
2.7 過硫酸鹽之催化	12
2.7.1 UV對過硫酸鹽的催化	14
2.7.2金屬對硫酸鹽的催化	14
2.7.3溫度對過硫酸鹽的催化	16
2.8影響過硫酸鹽催化之因素	17
2.8.1氧化劑與有機物間之不同莫耳比的影響	17
2.8.2 pH的影響	19
2.8.3 碳酸根及碳酸氫根的影響	21
第三章 實驗材料設備與方法	23
3.1實驗藥品	23
3.1.1染料廢水製備	23
3.1.2 Sodium Persulfate氧化劑試劑	23
3.1.3 Sodium Persulfate 殘餘分析藥品-硫代硫酸鈉滴定	23
3.2實驗設備	25
3.2.1反應器Photoreactor	25
3.2.2紫外光分光光度計(Ultra-Violet Spectrometer )	27
3.2.3其他實驗設備與材料	27
3.3實驗方法流程	27
3.4分析方法	28
3.4.1染料廢水降解分析	28
3.4.2過硫酸根殘餘量-硫代硫酸鈉滴定	30
第四章 實驗結果與討論	32
4.1溫度對染料及氧化劑自行分解影響	32
4.1.1溫度對orange II 降解	32
4.1.2溫度對過硫酸鈉的分解作用	33
4.2氧化劑/染料莫爾比 (NaPS/Dye) 及溫度控制對染料降解影響	34
4.2.1在20℃於不同NaPS/Dye莫爾比下降解染料影響	34
4.2.2在40℃於不同NaPS/Dye莫爾比下降解染料影響	35
4.2.3在60℃於不同NaPS/Dye莫爾比下降解染料影響	36
4.2.3.1在60℃於不同NaPS/Dye莫爾比下染料降解效率	36
4.2.3.2在60℃於不同NaPS/Dye莫爾比下降解動力常數	37
4.2.4於相同NaPS/Dye莫耳比在不同溫度下對染料降解影響	39
4.2.4.1於相同NaPS/Dye莫耳比在不同溫度下染料降解效率	39
4.2.4.2於相同NaPS/Dye莫爾比在不同溫度下降解動力常數	40
4.2.4.3於相同NaPS/Dye莫爾比在不同溫度下降解活化能	41
4.2.4.4於相同NaPS/Dye莫爾比在不同溫度下過硫酸鈉殘餘量探討	43
4.3溫度配合UV對染料及氧化劑自行分解影響	44
4.3.1溫度配合UV對orange II 降解	44
4.3.2溫度配合UV對過硫酸鈉的分解作用	45
4.4氧化劑/染料莫爾比 (NaPS/Dye) 及溫度控制並配合UV光對染料降解影響	46
4.4.1在20℃於不同NaPS/Dye莫爾比下配合UV光降解染料影響	46
4.4.2在40℃於不同氧NaPS/Dye莫爾比下配合UV光降解染料影響	47
4.4.2.1在40℃於不同氧NaPS/Dye莫爾比下染料降解效率	47
4.4.2.2在40℃於不同NaPS/Dye莫爾比配合UV光下降解動力常數	48
4.4.3在60℃於不同NaPS/Dye莫爾比下配合UV光降解染料影響	49
4.4.3.1在60℃於不同NaPS/Dye莫爾比下配合UV光染料降解效率	49
4.4.3.2在60℃於不同NaPS/Dye莫爾比配合UV光下降解動力常數	50
4.4.4溫度控制60℃於NaPS/Dye = 7.5及15配合UV光下降解階段反應探討	51
4.4.4.1在 60℃於NaPS/Dye = 7.5及15配合UV光下降解第一階反應	52
4.4.4.2在60℃於NaPS/Dye = 7.5及15配合UV光下降解第二階反應	53
4.4.5在60℃於NaPS/Dye =15配合UV光下降解不同濃度染料反應	54
4.4.5.1在60℃於NaPS/Dye =15配合UV光下降解不同濃度染料動力常數	55
4.4.5.2在60℃於NaPS/Dye =15配合UV光下降解不同濃度染料階段反應探討	56
4.4.5.3在60℃於NaPS/Dye =15配合UV光下降解不同濃度染料第一階反應	57
4.4.5.4在60℃於NaPS/Dye =15配合UV光下降解不同濃度染料第二階反應	58
4.4.6於相同氧化劑/染量莫爾濃度在不同溫度下配合UV光降解染料影響	59
4.4.6.1於相同氧化劑/染量莫爾濃度在不同溫度下配合UV光染料降解效率	59
4.4.6.2於相同氧化劑/染量莫爾濃度在不同溫度下配合UV光染料降解動力常數	60
4.4.6.3於相同氧化劑/染量莫爾濃度在不同溫度下配合UV光染料降解活化能	61
4.4.6.4於相同NaPS/Dye莫爾比在不同溫度下配合UV光過硫酸鈉殘餘量探討	62
4.5熱催化及熱配合UV光燈催化過硫酸鈉鹽降解染料探討	63
4.5.1熱催化及熱配合UV光燈催化過硫酸鈉鹽降解染料效率	63
4.5.2熱催化及熱配合UV光燈催化過硫酸鈉鹽降解染料常數	64
4.5.3熱催化及熱配合UV光燈催化過硫酸鈉鹽降解染料活化能探討	65
第五章結論與建議	67
Reference	69

List of Figure
Figure 1. The Chemical Structure of Dye	5
Figure 2. Mechanism of Diazotization	6
Figure 3. The Chemical Structure of Persulfate	10
Figure 4. The Chemical structure of Orange II	23
Figure 5. Schematic of Photoreactor	26
Figure 6. Schematic diagram of OrangeII degradation by NA2S2O8	28
Figure 7. Orange II absorbance vs. Wavelength for different concentrations.	29
Figure 8. Absorbance at 487nm vs. Orange II concentration.	29
Figure 9. Theoritical concentration vs. concentration defermined by Iodimetric titration method.	31
Figure 10. Effect of temperature on oxidation of Orange II without oxidatant at 20、40 and 60℃	33
Figure 11. Effect of temperature on decompostion of Na2S2O8 in DI water at 20、40 and 60℃	34
Figure 12. Comparison of decolorization efficiency in the different molar ratio of Na2S2O8 to OrangeII. [OrangeII] = 0.086mM;Temp = 20℃	35
Figure 13. Comparison of decolorization efficiency in the different molar ratio of Na2S2O8 to OrangeII. [OrangeII] = 0.086mM;Temp = 40℃	36
Figure 14. Comparison of decolorization efficiency in the different molar ratio of Na2S2O8 to OrangeII. [OrangeII] = 0.086mM;Temp = 60℃	37
Figure 15. Pseudo-first-order disappearance of OrangeII in the different molar ratio of Na2S2O8 to OrangeII.[OrangeII] = 0.086mM;Temp = 60℃	38
Figure 16. Comparison of decolorization efficiency at the different temperatures . [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	40
Figure 17. Pseudo-first-order disappearance of Orange II at the different temperatures . [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	41
Figure 18. Arrhenius Plots for Dye degradation. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	42
Figure 19. Persulfate decomposition in NaPS/Dye = 15 at the different temperatures. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	44
Figure 20. Effect of temperature combine UV on oxidation of OrangeII without oxidatant at 20℃、40℃ and 60℃	45
Figure 21. Effect of temperature and UV on decompose of Na2S2O8 without contaminant at 20℃、40℃ and 60℃	46
Figure 22. Comparison of decolorization efficiency in the different molar ratio of Na2S2O8 to OrangeII with UV.[OrangeII] = 0.086mM;Temp = 20℃	47
Figure 23. Comparison of decolorization efficiency i in the different molar ratio of Na2S2O8 to OrangeII with UV. [OrangeII] = 0.086mM;Temp = 40℃	48
Figure 24. Pseudo-first-order disappearance of OrangeII in the different molar ratio of Na2S2O8 to OrangeII with UV.[OrangeII] = 0.086mM;Temp = 40℃	49
Figure 25. Comparison of decolorization efficiency in NaPS/Dye molar ratio 15、7.5 and 1.5 at 60℃ with UV.	50
Figure 26. Pseudo-first-order disappearance of OrangeII in the different molar ratio of Na2S2O8 to OrangeII with UV.[OrangeII] = 0.086mM;Temp = 60℃	51
Figure 27. Comparison of pseudo-first-order disappearance of OrangeII in NaPS/Dye molar ratio 15 and 7.5 with UV. [OrangeII] = 0.086mM ;Temp = 60℃	52
Figure 28. Comparison of pseudo-first-order disappearance of OrangeII in NaPS/Dye molar ratio 15 and 7.5 with UV at phase of first. [OrangeII] = 0.086mM ;Temp = 60℃	53
Figure 29. Comparison of pseudo-first-order disappearance of OrangeII in NaPS/Dye molar ratio 15 and 7.5 with UV at phase of second. [OrangeII] = 0.086mM ;Temp = 60℃	54
Figure 30. Comparison of decolorization efficiency in the different dye concentration with UV. [ Na2S2O8] = 1.28 mM ;Temp = 60℃	55
Figure 31. Pseudo-first-order in the different concentratrion of dye with UV.[ NaPS/Dye = 15];Temp = 60℃	56
Figure 32. Comparison of pseudo-first-order in the different concentratrion of dye with UV.[ NaPS/Dye = 15];Temp = 60℃.	57
Figure 33. Comparison of pseudo-first-order in the different concentratrion of Orange II with UV at phase of first. [ NaPS/Dye = 15] ;Temp = 60℃	58
Figure 34. Comparison of pseudo-first-order in the different concentratrion of Orange II with UV at phase of second. [ NaPS/Dye = 15] ;Temp = 60℃	59
Figure 35. Comparison of decolorization efficiency at the different temperatures  with UV . [Orange II] = 0.086mM;[ Na2S2O8] = 1.28 mM	60
Figure 36. Pseudo-first-order disappearance of Orange II at the different temperatures with UV. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	61
Figure 37. Arrhenius Plots for Dye degradation at the different temperatures with UV. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	62
Figure 38. Persulfate decomposition in NaPS/Dye = 15 with UV at the different temperatures. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	63
Figure 39. Comparison of decolorization efficiency with thermal in UV and non-UV system. [OrangeII] = 0.086mM; [ Na2S2O8] = 1.28 mM;Temp = 60℃	64
Figure 40. Pseudo-first-order disappearance of Orange II with thermal in UV and non-UV system. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM; Temp = 60℃	65
Figure 41. Arrhenius Plots for Dye degradation with thermal in UV and non-UV system. [OrangeII] = 0.086mM;[ Na2S2O8] = 1.28 mM	66


List of Table
Table 1. Chromophore	5
Table 2. Physical and Chemical Properties of Persulfates	11
Table 3. Standard Redox Potential of Selected Oxidants(21, 35)	12
Table 5.Reagen used in this study	25
Table 6. Degradation of Dye at Temperature of 60℃ as a Function of Oxidant/Contaminant Molar Ratio	39
Table 7.Degradation of Dye at an Oxidant/Contaminant Molar Ration of 15/1 as a Funtion of Temperature	43
Table 7. Degradation of Dye at Temperature of 40℃with UV as a Function of Oxidant/Contaminant Molar Ratio	49
Table 8. Degradation of Dye at Temperature of 60℃with UV as a Function of Oxidant/Contaminant Molar Ratio	51
Table 9.Dye Degradation at an Oxidant/Contaminant Molar Reaction 15/1 as a Funtion of Temperature with UV	62

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