高級氧化處理(Advanced oxidation processes, AOPs)實際在環境上之應用及過去文獻討論中已相當成熟，然而如何找出最適合的反應條件以及高利用率，並結合多種程序，包括單用過氧化氫、紫外線，以及UV/H2O2、UV/SPS、Fenton、Photo-Fenton等程序比較，過去並無太多研究進行比較，故本研究將四環素水溶液經不同程序反應後，比較處理前後四環素降解效率。
    實驗結果顯示，四種程序在60分鐘的反應後，皆對四環素有明顯的降解效果，然 Photo-Fenton系統之去除效率為四種程序裡最佳的。在有使用紫外光照射的程序中，皆有光強度愈高去除率愈高的趨勢，但是因為污染物濃度條件未造成明顯光遮蔽效應，因此去除率差異不大。污染物濃度愈高在不同的程序皆有去除率愈低的趨勢，高濃度的四環素會降低UV光的穿透能力，以及降低鐵離子與氧化劑的碰撞。四種程序之氧化劑濃度設定皆無產生明顯的自身反應，因此氧化劑濃度愈高皆會使得自由基產生的效率愈高，間接導致四環素去除率提升。鐵離子在Fenton系統中有催化氧化劑的作用，因此愈高的鐵離子能增加與氧化劑的碰撞而提高自由基的產生，能更有效率的降解四環素。在降解四環素的四種不同程序中，pH是一個很關鍵的影響因子，因為四環素是兩性有機物，在不同的pH條件有不同的解離形式，實驗解果顯示愈高的pH有愈高的四環素去除率，但是在pH大於11時，會因為氧化劑自身的解離使得去除率下降，因此UV/H2O2系統以及UV/SPS系統pH=9為最佳的操作條件。
	電能量損耗效益(EE/O)於氧化劑濃度愈高之情況下所需耗能愈低，顯示愈高的氧化劑濃度可以增加自由基產生的效率，能在更短的時間達到相同的去除率，反應時間縮短因此電耗能降低。

The application of advanced oxidation treatment (AOPs) in the environment and the discussion of past literature are quite mature. However, how to find out the most suitable reaction conditions and high utilization rate, and combine a variety of procedures, including single-use oxidation process, ultraviolet line, and UV/H2O2、UV/SPS、Fenton、Photo-Fenton.
The experimental results show that the four procedures have a significant degradation effect on tetracycline after 60 minutes of reaction, but the removal efficiency of the Photo-Fenton system is the best among the four procedures. In the procedures that use ultraviolet light, the higher the light intensity, the higher the removal rate. However, because the pollutant concentration conditions did not cause a significant light shielding effect, the removal rate has little difference. The higher the concentration of pollutants, the lower the removal rate in different procedures. High concentrations of tetracycline will reduce the penetration of UV light and reduce the collision of iron ions with oxidants. The oxidant concentration settings of the four programs have no obvious self-reaction. Therefore, the higher the oxidant concentration, the higher the efficiency of free radical generation, which indirectly leads to the increase in the removal rate of tetracycline. Iron ions act as a catalytic oxidant in the Fenton system. Therefore, higher iron ions can increase collisions with oxidants and increase the generation of free radicals, which can degrade tetracycline more efficiently. Among the four different processes for the degradation of tetracycline, pH is a very critical factor, because tetracycline is an amphoteric organic matter, and has different dissociation forms under different pH conditions. The experimental results show that the higher the pH, the higher the removal of tetracycline. However, when the pH is greater than 11, the removal rate will decrease due to the dissociation of the oxidant itself. Therefore, the UV/H2O2 system and the UV/SPS system pH=9 are the best operating conditions.
The more oxidant doze requires less energy to produce oxidants results in better energy efficiency, which shows that the higher the oxidant concentration can increase the efficiency of free radical generation, the same removal rate can be achieved in a shorter time, the reaction time is shortened, and the power consumption is reduced.

目錄	I
第一章 前言	IV
1-1. 研究動機	1
1-2. 研究目的	2
第二章 文獻回顧	4
2-1. 抗生素	4
2-2. 四環素物化特性	5
2-3. 高級氧化程序	7
2-4. 過氧化氫特性及應用	11
2-5. 過硫酸鹽特性及應用	12
2-6. 硫化亞鐵特性及應用	14
2-7. 光化學反應及動力模式	15
2-7-1.無直接光解反應(He et al., 2014)	15
2-7-2.有直接光解反應(Baeza et al., 2011)	16
2-8.  UV/H2O2 反應機制及相關研究	17
2-8-1. pH之影響	19
2-8-2. H2O2 劑量之影響	21
2-8-3. 污染物濃度之影響	22
2-8-4. UV光之影響	23
2-9. UV/SPS 反應機制及相關研究	25
2-9-1. pH之影響	30
2-9-2. H2O2 劑量之影響	31
2-9-3. 污染物濃度之影響	32
2-9-4. UV光強度之影響	32
2-10. Fenton及Photo-Fenton反應機制及相關研究	34
2-10-1. Fenton反應機制	34
2-10-2. Photo-Fenton	35
第三章 研究方法與材料	37
3-1. 實驗設備	37
3-2. 實驗藥品及配比	38
3-2-1. 實驗藥品	38
3-2-2. 四環素水溶液製備 (400 mg/L)	39
3-2-3. 過氧化氫氧化劑儲存溶液製備	39
3-2-4. 硫酸亞鐵儲存溶液製備	39
3-2-5. 氧化劑殘餘量分析-碘定量法	39
3-3. 實驗裝置	39
3-4. 實驗方法	42
3-4-1.實驗架構	42
3-4-2.實驗流程	43
3-5. 分析測定方法	44
3-5-1. HPLC分析	44
3-5-2. 吸光度分析	45
第四章 結果與討論	46
4-1. 背景實驗	46
4-1-1. 單用氧化劑實驗	46
4-1-2. 直接光解實驗	47
4-2. 以UV/H2O2 系統降解含四環素水溶液之探討	49
4-2-1. 光強度效應	49
4-2-2. 污染物濃度效應	51
4-2-3. 氧化劑濃度效應	54
4-2-4. pH效應	56
4-3. 以UV/SPS 系統降解含四環素水溶液之探討	59
4-3-1. 光強度效應	59
4-3-2. 污染物濃度效應	62
4-3-3. 氧化劑濃度效應	64
4-3-4. pH效應	66
4-4. 以Fenton及Photo-Fenton程序降解含四環素水溶液之探討	70
4-4-1. 光強度效應	71
4-4-2. 污染物濃度效應	72
4-4-3. 氧化劑濃度效應	76
4-4-4. 鐵離子濃度效應	79
4-4-5. pH效應	83
4-5. 不同系統處理含四環素水溶液比較	88
4-5-1. 光強度效應	89
4-5-2. 污染物濃度效應	89
4-5-3. 氧化劑濃度效應	90
4-5-4. pH效應	91
第五章 結論與建議	93
5-1. 結論	93
5-2. 建議	96
參考文獻(英文)	97
參考文獻(中文)	103


圖目錄
圖2- 1 OECD國家管理水中藥物殘留現況	4
圖2- 2 四環素在不同pH水溶液環境中的物種分布。(Zhang et al., 2020)	6
圖2- 3 四環素在不同pKa之分子結構。(Zhang et al., 2020)	6
圖2- 4 用於去除污染物的化學處理方法概述	7
圖2- 5 藉由UV光催化氧化劑並進行污染物之降解作用 (Xu et al., 2016)	9
圖2- 6 由不同高級氧化程序產生氫氧自由基之機制 (Cheng et al., 2016)	9
圖2- 7 過氧化氫於不同pH值之成分分布 (申永順。1992)	11
圖2- 8 UV/H2O2 去除 EDCs 機制圖 (Zhang et al., 2014)	18
圖2- 9 UV/PS 反應機制(Xu et al., 2020)	25
圖2- 10 MPUV/PMS 反應機制(Ao et al., 2019)	25
圖2- 11 不同程序之氧化劑花費與電能量比較圖 (Antoniou et al., 2015)	33
圖2- 12 Fenton與UV照射時發生的反應(Juan M et al.2018)	36
圖3- 1 光反應槽示意圖	41
圖3- 2 以紫外光測定計測定UVC燈管之光強度	41
圖3- 3 實驗架構圖	42
圖3- 4 四環素檢量線	44
圖3- 5 四環素於不同pH值水溶液環境之吸光度分析	45
圖4- 1 H2O2 only直接氧化TC之去除率變化圖	47
圖4- 2 SPS only直接氧化TC之去除率變化圖	47
圖4- 3 UVonly不同光pH降解TC之變化圖	48
圖4- 4 UVonly不同光強度降解TC之變化圖	49
圖4- 5 UV/H2O2系統中不同光強度降解TC之變化圖	50
圖4- 6 UV/H2O2系統中不同光強度降解TC之反應動力常數變化圖	50
圖4- 7 UV/H2O2系統中不同光強度降解TC之動力學線性圖	50
圖4- 8 UV/H₂O₂ 系統中不同光強度之電耗能變化圖	51
圖4- 9 UV/ H₂O₂系統中不同TC初始濃度降解變化圖	52
圖4- 10 UV/ H₂O₂系統中不同TC初始濃度之反應動力常數變化圖	52
圖4- 11 UV/ H₂O₂系統中不同TC初始濃度之動力學線性圖	53
圖4- 12 UV/H₂O₂ 系統中不同污染物濃度之電耗能變化圖	53
圖4- 13 UV/ H₂O₂系統中不同氧化劑濃度降解TC之變化圖	54
圖4- 14 UV/ H2O2系統中不同氧化劑濃度降解TC之反應動力常數變化圖	55
圖4- 15 UV/H2O2系統中不同氧化劑濃度降解TC之動力學線性圖	55
圖4- 16 UV/H₂O₂ 系統中不同氧化劑濃度之電耗能變化圖	56
圖4- 17 UV/H₂O₂系統中不同pH水溶液環境降解TC之變化圖	57
圖4- 18 UV/H₂O₂系統中不同pH水溶液環境降解TC之反應動力常數變化圖	57
圖4- 19 UV/H2O2系統中不同pH水溶液環境降解TC之動力學線性圖	58
圖4- 20 UV/H₂O₂ 系統中不同pH之電耗能變化圖	59
圖4- 21 UV/SPS系統中不同光強度環境降解TC之變化圖	60
圖4- 22 UV/SPS系統中不同光強度降解TC之反應動力常數變化圖	60
圖4- 23 UV/SPS系統中不同光強度降解TC之動力學線性圖	61
圖4- 24 UV/SPS系統中不同光強度之電耗能變化圖	62
圖4- 25 UV/SPS系統中不同TC初始濃度降解變化圖	63
圖4- 26 UV/SPS系統中不同TC濃度之反應動力常數變化圖	63
圖4- 27 UV/SPS系統中不同TC濃度之動力學線性圖	63
圖4- 28 UV/SPS系統中不同TC初始濃度之電耗能變化圖	64
圖4- 29 UV/SPS系統中不同氧化劑濃度降解TC之變化圖	65
圖4- 30 UV/SPS系統中不同氧化劑濃度降解TC之反應動力常數變化圖	65
圖4- 31 UV/SPS系統中不同氧化劑濃度降解TC之動力學線性圖	66
圖4- 32 UV/SPS系統中不同氧化劑濃度之電耗能變化圖	67
圖4- 33 UV/SPS系統中不同pH水溶液環境降解TC之變化圖	68
圖4- 34 UV/SPS系統中不同pH水溶液環境降解TC之反應動力常數變化圖	69
圖4- 35 UV/SPS系統中不同pH水溶液環境降解TC之動力學線性圖	69
圖4- 36 UV/SPS系統中不同pH之電耗能變化圖	70
圖4- 37 Photo-Fenton系統中不同光強度降解TC之變化圖	71
圖4- 38 Photo-Fenton系統中不同光強度降解TC之反應動力常數變化圖	71
圖4- 39 Photo-Fenton系統中不同光強度降解TC之動力學線性圖	72
圖4- 40 Photo-Fenton系統中不同光強度之電耗能變化圖	72
圖4- 41 Fenton系統中不同TC初始濃度降解變化圖	73
圖4- 42 Fenton系統中不同TC初始濃度之反應動力常數變化圖	74
圖4- 43 Fenton系統中不同TC初始濃度之動力學線性圖	74
圖4- 44 Photo-Fenton系統中不同TC初始濃度降解變化圖	75
圖4- 45 Photo-Fenton系統中不同TC初始濃度之反應動力常數變化圖	75
圖4- 46 Photo-Fenton系統中不同TC初始濃度之電耗能變化圖	76
圖4- 47 Fenton系統中不同氧化劑濃度降解TC之變化圖	77
圖4- 48 Fenton系統中不同氧化劑濃度降解TC之反應動力常數變化圖	77
圖4- 49 Fenton系統中不同氧化劑濃度降解TC之動力學線性圖	77
圖4- 50 Photo-Fenton系統中不同氧化劑濃度降解TC之變化圖	78
圖4- 51 Photo-Fenton系統中不同氧化劑濃度降解TC之反應動力常數變化圖	78
圖4- 52 Photo-Fenton系統中不同氧化劑濃度之電耗能變化圖	79
圖4- 53 Fenton系統中不同鐵離子濃度降解TC之變化圖	80
圖4- 54 Fenton系統中不同鐵離子濃度降解TC之反應動力常數變化圖	81
圖4- 55 Fenton系統中不同鐵離子濃度降解TC之動力學線性圖	81
圖4- 56 Photo-Fenton系統中不同鐵離子濃度降解TC之變化圖	82
圖4- 57 Photo-Fenton系統中不同鐵離子濃度降解TC之反應動力常數變化圖	82
圖4- 58 Photo-Fenton系統中不同鐵離子濃度降解TC之動力學線性圖	83
圖4- 59 Photo-Fenton系統中不同鐵離子濃度之電耗能變化圖	83
圖4- 60 Fenton系統中不同pH水溶液環境降解TC之變化圖	84
圖4- 61 Fenton系統中不同pH水溶液環境降解TC之反應動力常數變化圖	85
圖4- 62 Fenton系統中不同pH水溶液環境降解TC之動力學線性圖	85
圖4- 63 Photo-Fenton系統中不同不同pH水溶液環境降解TC之變化圖	86
圖4- 64 Photo-Fenton系統中不同pH降解TC之反應動力常數變化圖	87
圖4- 65 Photo-Fenton系統中不同pH之電耗能變化圖	87
圖4- 66 三種AOP主要反應機制圖（Qiu et al., 2019）	88
圖4- 67不同AOPs探討光強度效應	89
圖4- 68不同AOPs探討污染物濃度效應	90
圖4- 69以UV/H₂O₂ & UV/SPS 程序探討氧化劑濃度效應	91
圖4- 70 以Fenton & Photo-Fenton探討氧化劑濃度效應	91
圖4- 71以UV/H₂O₂ & UV/SPS 程序探討pH效應	92
圖4- 72以Fenton & Photo-Fenton探討pH效應	92
 
表目錄
表2- 1四環素物化特性	5
表2- 2常見的氧化劑標準還原電位 (Latimer., 1952)	10
表2- 3過氧化氫之物化特性	12
表2- 4過硫酸鹽之物化特性	13
表2- 5硫酸亞鐵之物化特性	14
表2- 6有機物存在UV/S2O82-時之反應機制 (Xie et al., 2015)	28
表3- 1本研究所需各項實驗設備之來源與目的	37
表3- 2實驗藥品	38
表3- 3使用HPLC於四環素水溶液之操作條件	44
表4- 1不同光強度之貢獻率比較	51
表4- 2 UV/ H2O2系統中不同氧化劑濃度之貢獻率	56
表4- 3 UV/ H₂O₂系統中不同pH水溶液環境之貢獻率	58
表4- 4 UV/SPS 系統中不同光強度之貢獻率	61
表4- 5 UV/SPS 系統中不同氧化劑濃度之貢獻率	66
表4- 6 UV/SPS 系統中不同pH水溶液環境之貢獻率	70

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