臺灣博碩士論文加值系統

　　本研究目的為利用高級氧化處理程序(Advanced Oxidation Processes, AOPs)對20 ppm磺胺噻唑(Sulfathiazole, STZ)進行降解效果與礦化效果之探討，藉由改變pH值與氧化劑劑量找出降解與礦化STZ之最佳化程序，並分析臭氧與過氧化氫之殘留濃度變化。研究使用AOPs分別為O3, UV/O3, O3/H2O2, UV/H2O2, O3/Na2S2O8, UV/Na2S2O8, UV/O3/H2O2及UV/O3/Na2S2O8程序，此外，於UV/O3, UV/Na2S2O8及UV/O3/Na2S2O8程序在pH 7與pH 9分別添加1 wt%與3.5 wt%鹽度，探討模擬海水環境下對STZ之降解效率與礦化效率的影響。
　　研究結果顯示，UV/O3/Na2S2O8程序於pH 7具有最佳降解效率以及最佳礦化效率，皆為99%，並經擬一階動力學計算出在UV/O3/Na2S2O8程序於pH 5時有最大之反應速率常數0.0835 min-1。臭氧殘留濃度分析方面，臭氧於鹼性環境下比在酸性環境下不穩定，故殘留濃度較低。過氧化氫殘留濃度分析方面，過氧化氫於鹼性環境時分解迅速，殘留濃度較低。模擬海水鹽度實驗中，於pH 9添加3.5 wt%鹽度至UV/Na2S2O8程序時礦化效率明顯降低。本研究於pH 5時對O3/H2O2與UV/O3/H2O2程序進行過氧化氫濃度效應實驗，找出過氧化氫最佳添加量；在O3/H2O2程序，過氧化氫最佳添加量為5 mM，對STZ有最佳礦化效率69%，在UV/O3/H2O2程序，過氧化氫最佳添加量為2.5 mM，對STZ有最佳降解效率與礦化效率分別為99%與87%。
　　活性物種捕捉劑實驗發現STZ在UV/O3程序的反性活性物種為氫氧自由基(Hydroxyl Radical, HO•)，UV/O3/Na2S2O8程序的反應活性物種為氫氧自由基及陰離子硫酸自由基(Sulfate Radical, SO4－•)，且於pH 9環境下所含之氫氧自由基與陰離子硫酸自由基數量較pH 5與pH 7多。

The purpose of this study was to investigate the removal efficiency and mineralization efficiency of Sulfathiazole (STZ) by advanced oxidation processes included O3, UV/O3, O3/H2O2, O3/Na2S2O8, UV/H2O2, UV/Na2S2O8, UV/O3/H2O2 and UV/O3/Na2S2O8. The effects of pH on the removal efficiency and mineralization efficiency of STZ were investigated, and the changes of residual ozone concentration and residual hydrogen peroxide concentration were analyzed. Besides, 1 wt% and 3.5 wt% salinity were set up in UV/O3, UV/Na2S2O8 and UV/O3/Na2S2O8 processes at pH 7 and pH 9 to simulate as seawater condition.
The UV/O3/Na2S2O8 process at pH 7 showed the best STZ removal efficiency and mineralization efficiency both 99%. The pseudo-first-order rate constant of STZ in the UV/O3/Na2S2O8 system at pH 5 was 0.0835 min-1. Residual ozone concentration was lower in alkaline conditions which ozone was less stable in alkaline conditions than in acidic and neutral conditions. Residual hydrogen peroxide concentration was lower in alkaline conditions while the hydrogen peroxide could be decomposed easily in alkaline conditions than in acidic and neutral conditions. 3.5 wt% salinity in UV/Na2S2O8 process at pH 9 decreased STZ mineralization efficiency from 85% to 51%. The effects of hydrogen peroxide concentration at pH 5 were performed in the O3/H2O2 and UV/O3/H2O2 systems. The best mineralization efficiency of STZ in O3/H2O2 process was 69% with 5 mM hydrogen peroxide concentration. The best removal efficiency and mineralization efficiency of STZ in UV/O3/H2O2 process ware 99% and 87% with 2.5 mM hydrogen peroxide concentration.
The experimental results of active species trapping revealed that hydroxyl radicals (HO•) played a major role in the UV/O3 process and the major active species were hydroxyl radicals and sulfate radicals (SO4－•) in the UV/O3/Na2S2O8 system. Moreover, the concentration of hydroxyl radicals and sulfate radicals was higher at pH 9 than at pH 5 and pH 7.

摘要 I
Abstract III
致謝 V
目錄 VI
表目錄 IX
圖目錄 X
第一章、緒論 1
1.1 研究動機 1
1.2 研究目的及內容 2
第二章、文獻回顧 3
2.2 高級氧化處理程序 5
2.2.1 臭氧基本性質及氧化原理 7
2.2.2 紫外光氧化原理 12
2.2.3 過氧化氫基本性質及氧化原理 13
2.2.4 過硫酸鈉基本性質及氧化原理 13
2.3 臭氧結合紫外光、過氧化氫與過硫酸鹽程序 14
2.3.1 UV/O3程序原理 14
2.3.2 O3/H2O2程序原理 15
2.3.3 O3/Persulfate程序原理 16
2.4 紫外光結合過氧化氫及過硫酸鹽程序 19
2.4.1 UV/H2O2程序原理 19
2.4.2 UV/Persulfate程序原理 20
2.5 UV/O3結合過氧化氫及過硫酸鹽程序 22
2.5.1 UV/O3/H2O2程序原理 22
2.5.2 UV/O3/Persulfate程序原理 24
第三章、實驗方法 27
3.1 實驗藥品與儀器 27
3.2 研究架構 29
3.3 分析方法 30
3.3.1 STZ濃度分析 30
3.3.2 總有機碳濃度分析 32
3.3.3 臭氧流量分析 33
3.3.4 殘留臭氧濃度分析 34
3.3.5 殘留過氧化氫濃度分析 35
3.4 實驗流程與操作變因 36
3.4.1 O3程序流程 36
3.4.2 UV/O3程序流程 36
3.4.3 O3/Ox程序流程 37
3.4.4 UV/Ox程序流程 38
3.4.5 UV/O3/Ox程序流程 39
3.5 氧化程序實驗 41
3.5.1 UV直接光解實驗 43
3.5.2 O3直接氧化實驗 43
3.5.3 UV/O3氧化實驗 43
3.5.4 O3/H2O2氧化實驗 44
3.5.5 O3/Na2S2O8氧化實驗 44
3.5.6 UV/H2O2氧化實驗 45
3.5.7 UV/Na2S2O8氧化實驗 45
3.5.8 UV/O3/H2O2氧化實驗 46
3.5.9 UV/O3/Na2S2O8氧化實驗 46
3.5.10 再現性實驗 47
3.5.11 活性物種捕捉劑實驗 47
3.5.12 模擬海水鹽度氧化實驗 48
3.5.13 反應動力學模擬 49
3.5.14 單位電能數據分析 49
第四章、結果與討論 50
4.1 UV直接光解實驗數據分析 50
4.2 O3氧化實驗數據分析 51
4.3 UV/O3氧化實驗數據分析 54
4.4 O3/H2O2氧化實驗數據分析 56
4.4.1 O3/H2O2程序之H2O2劑量效應數據分析 56
4.4.2 O3/H2O2程序之pH值效應數據分析 59
4.5 O3/Na2S2O8氧化實驗數據分析 63
4.6 UV/H2O2氧化實驗數據分析 66
4.7 UV/Na2S2O8氧化實驗數據分析 69
4.8 UV/O3/H2O2氧化實驗數據分析 70
4.8.1 UV/O3/H2O2程序之H2O2劑量效應數據分析 70
4.8.2 UV/O3/H2O2程序之pH值效應數據分析 73
4.9 UV/O3/Na2S2O8氧化實驗數據分析 76
4.10 模擬海水鹽度氧化實驗數據分析 79
4.11 反應動力學模擬數據分析 90
4.12 能量消耗及成本數據分析 97
4.13 活性物種捕捉劑實驗數據分析 102
4.13.1 O3程序活性物種捕捉劑實驗數據分析 102
4.13.2 UV/O3程序活性物種捕捉劑實驗數據分析 105
4.13.3 UV/O3/Na2S2O8程序活性物種捕捉劑實驗數據分析 108
第五章、結論與建議 111
5.1 結論 111
5.2 建議 113
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