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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 蔣本基 | |
dc.contributor.author | Tzu-Yu Liu | en |
dc.contributor.author | 劉子瑜 | zh_TW |
dc.date.accessioned | 2021-06-15T05:07:04Z | - |
dc.date.available | 2020-07-23 | |
dc.date.copyright | 2010-07-27 | |
dc.date.issued | 2010 | |
dc.date.submitted | 2010-07-26 | |
dc.identifier.citation | Reference
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/46398 | - |
dc.description.abstract | 摘要
甲芬納酸 (Mefenamic acid )為一種非常廣泛使用的非類固醇抗發炎藥物,甲芬納酸為雙酚胺的衍生物物種之一,雙酚胺已被歐盟列為首要重點污染物,主要原因為雙酚胺相關衍生物暴露於水體環境中可造成部分的毒性危害,許多研究調查指出甲芬納酸可被許多污水處理廠檢測出微量濃度,主要原因為甲芬納酸無法完全被污水處理廠有效去除。因此,評估微量甲芬納酸存在環境水體之問題應被重視。 本研究目的在於評估臭氧及臭氧/紫外光處理程序對甲芬納酸去除的影響。評估不同的操作條件,例如:臭氧劑量、pH、UV紫外光、水中添加鹼度及腐殖酸對甲芬納酸去除影響之調查。更進一步研究,臭氧副產物生成潛勢。同時發展甲芬納酸降解預測模式,可決定反應動力常數與解釋甲芬納酸降解機制。最後利用最佳化設計結合反應取面法決定實驗最佳化設計之參數。 研究結果顯示出利用臭氧及臭氧/紫外光處理程序可有效的去除甲芬納酸。在臭氧及臭氧/紫外光處理程序中,提高臭氧劑量與降低pH可明顯提高甲芬納酸去除率。水中添加基質,例如:腐殖酸,會降低甲芬納酸去除率。甲芬納酸降解預測模式,在臭氧/紫外光處理程序中,成功可決定甲芬納酸反應速率常數。更進一步研究指出,在紫外光處理程序中,臭氧副產物醛類生成濃度隨操作條件pH增加而增加生成量,主要原因為較有多氫氧自由基,容易將有機物質氧化成小分子醛類物質。最後利用反應取面法可得知影響甲芬納酸降解的重要參數為臭氧劑量、pH、反應時間與腐殖酸添加濃度。 | zh_TW |
dc.description.abstract | Mefenamic acid (MEF) is a widely used anti-inflammatory drug. MEF is a diphenylamine derivative pollutant (DPA) which is the third compound in the European Union list of priority pollutants, because of its harmful properties with numeral toxic derivatives being observed in the aquatic environment. Many investigations have revealed that MEF can not be completely removed by conventional sewage treatment plants (STP) and was detected in STP effluents at trace levels. Therefore, the presence of MEF in the aquatic environment should be assessed critically.
The objective of this study was to evaluate the removal of MEF using ozonation and O3/UV processes. The effect of various operating parameters including ozone dose, pH, light intensity (UV), alkalinity, and humic acid on the removal of MEF in ozonation and O3/UV processes was investigated. In addition, the formation of ozonation by-products was also studied. Meanwhile, a simplified model based on MEF decomposition was developed to determine the reaction rate constants of MEF and to interpret the degradation of MEF. Finally, a response surface method was used to evaluate the effect of operation parameters on the degradation efficiency of MEF by ozonation and O3/UV processes. The results show that ozonation and O3/UV processes were efficient in degrading MEF. In both processes, increase of ozone dosage and decrease of pH enhanced MEF removal. The presence of humic acid can reduce MEF removal also. The MEF degradation model can predict the MEF degradation well. The reaction rate constants of MEF can be determined in a second order reaction. In addition, the aldehyde concentration increased with increasing pH in the ozonation process, which indicated the involvement of hydroxyl radical in aldehyde formation. By using the response surface method, it was found that MEF degradation was sensitive to factors such as ozone concentration, pH, reaction time, and humic acid concentration. | en |
dc.description.provenance | Made available in DSpace on 2021-06-15T05:07:04Z (GMT). No. of bitstreams: 1 ntu-99-R97541121-1.pdf: 1295150 bytes, checksum: 5dcc4693053c0cbbb97f7c5bdcfe1ab0 (MD5) Previous issue date: 2010 | en |
dc.description.tableofcontents | Contents
致謝 I Abstract II 中文摘要 IV Contents VI List of Figures IX List of Tables XIII Chapter 1 Introduction 1-1 1-1 Background 1-1 1-2 Objectives 1-3 Chapter 2 Literature Reviews 2-1 2-1 The Characteristics of Pharmaceuticals and Personal Care Products 2-1 2-2 The Characteristics of Mefenamic acid 2-1 2-3 NSAID Analytical Methods 2-5 2-4 Ozonation and Ozonation By-Products Formation 2-13 2-4-1 Ozonation 2-18 2-4-2 O3/UV Process 2-22 2-4-3 Ozonation By-Products formation 2-23 2-5 Predictive Model of Ozone Decay and Ozonation By-Products Formation 2-25 2-5-1 Ozonation Decay 2-25 2-5-2 Ozonation by-products formation 2-26 Chapter 3 Materials and Methods 3-1 3-1 Research Flowchart 3-1 3-2 Synthetic Water Preparation 3-2 3-3 Methods 3-2 3-3-1 Experimental Design 3-2 3-3-2 Establish NSAIDs Analytical Method 3-4 3-3-3 Ozonation and Advanced Oxidation Process 3-9 3-3-4 Analytical Methods 3-15 3-3-4-1 Water Quality Parameters 3-15 3-3-4-2 Ozonation and O3/UV By-Products 3-16 3-3-4 Risk Assessment 3-18 Chapter 4 Results and Discussion 4-1 4-1 Ozonation Process 4-1 4-1-1 Effect of Different Ozone Dosages Levels 4-1 4-1-2 Effect of Different pH Value Levels 4-6 4-2 O3/UV Process 4-12 4-2-1 Effect of Different pH Value Levels 4-12 4-2-2 Ozonation Process compare to O3/UV Process 4-17 4-3 Effect of Matrix in Ozonation and O3/UV Process 4-25 4-3-1 Effect of humic acid addition 4-25 4-3-2 Effect of alkalinity addition 4-28 4-4 Simulative model for MEF degradation during ozonation and O3/UV process 4-32 4-5 Ozoantion and By-Products 4-35 4-5-1 Ozonation By-Products formation 4-35 4-5-2 Predictive Ozonation By-Products formation Model 4-35 4-5-3 Risk Assessment 4-36 4-6 Optimum Operation conditions for Mefenamic acid Degradation 4-38 Chapter 5 Conclusions and Recommendations 5-1 5-1 Conclusions 5-1 5.2 Recommendations 5-3 Reference R-1 Appendix A-1 List of Figures Figure 2-2-1 The chemical structures of formal DPA 2-3 Figure 2-3-1 Common features of analytic methods considered for determination of pharmaceuticals 2-6 Figure 2-4-1 The reaction mechanism of aqueous ozone with organic matter (M) in the solutes 2-18 Figure 2-4-2 Scheme of Criegee mechanism 2-20 Figure 2-4-3 The reaction mechanism of ozone and aromatic compound 2-20 Figure 2-4-4 Reaction of hydroxyl radical with organic pollutant (P) leading to a great diversity of oxidized compounds 2-21 Figure 2-4-5.Schematic representation of the mechanism of phenol oxidation with ozone 2-24 Figure 3-1 Research flowchart 3-1 Figure 3-3-1 Flowchart of experiments to determine the reaction mechanism 3-3 Figure 3-3-2 Flowchart of experiments to analyze mefenamic acid process 3-4 Figure 3-3-3 GC/EI-MS system 3-5 Figure 3-3-4 Flowchart of ozonation and O3/UV process 3-9 Figure 3-3-5 The experiment apparatus of ozone batch reactor 3-13 Figure 3-3-6 The experiment apparatus of ozone semi-batch reactor 3-14 Figure 4-1-1. Time dependent of the degradation of MEF during the ozonation at various levels of ozone dose. system: (a) (●): 0.2, (■): 0.5, and (▲): 5.0 mg L-1 (Experimental conditions: CMEF0: 0.5 mg L-1 and pH 7); (b) (●): 0.2, (■): 1.5, and (▲): 3.5 mg L-1 (◆): 5.0 mg L-1 (Experimental conditions: CMEF0: 0.5 mg L-1 and pH 4) 4-3 Figure 4-1-2 Time dependent of the degradation of TOC during the ozonation at various levels of ozone dose. system: (a) (○): 0.5, (□):1.5, and (△): 15 mg L-1 (Experimental conditions: CMEF0: 1.0 mg L-1 and pH 7); (b) (○): 0.5, (□):1.5, and (△): 15 mg L-1 (Experimental conditions: CMEF0: 1.0 mg L-1 and pH 4) 4-5 Figure 4-1-3 Time dependent of the degradation of MEF during the ozonation at various levels of pH value. system: (a) (●): pH 4, (■): pH 7, and (▲): pH 9 (Experimental conditions: CMEF0: 0.5 mg L-1, Ozone dose: 0.2 mg L-1 ); (b) (●): pH 4, (■): pH 7, and (▲): pH 9 (Experimental conditions: CMEF0: 0.5 mg L-1, and Ozone dose: 0.7 mg L-1 ) 4-8 Figure 4-1-4 MEF removal efficiencies at various ozone dosages: (a) Ozone: 0.2 mg L-1; (b) Ozone: 3.5mg L-1; (c) Ozone: 5.0 mg L-1 (Experimental conditions: CMEF0: 0.5 mg L-1; reaction time: 60 min) 4-9 Figure 4-1-5 Time dependent of the degradation of TOC during the ozonation at various pH values. system: (a) (○): pH 4, (□): pH 7, and (△): pH 9 (Experimental conditions: CMEF0: 1.0 mg L-1 and ozone dose: 0.5 mg L-1); (b) (○): pH 4, (□): pH 7, and (△): pH 9 (Experimental conditions: CMEF0: 1.0 mg L-1 and and Ozone dose: 1.5 mg L-1) 4-11 Figure 4-2-1. Time dependent of the degradation of MEF during the O3/UV process at various pH values. system: (a) (●): pH 4, (■): pH 7, and (▲): pH 9 (Experimental conditions: CMEF0: 0.5 mg L-1 and Ozone dose: 0.2 mg L-1); (b) (●): pH 4, (■): pH 7, and (▲): pH 9 (Experimental conditions: CMEF0: 0.5 mg L-1 and Ozone dose: 0.7 mg L-1) 4-14 Figure 4-2-2 Time dependent of the degradation of TOC during the O3/UV process at various pH values. (a) Ozone dose: 0.5 mg L-1, (b) Ozone dose: 1.5 mg L-1, and (c) Ozone dose: 15 mg L-1 (●): pH 4, (■): pH 7, and (▲): pH 9 (Experimental condition: CMEF0: 1.0 mg L-1) 4-16 Figure 4-2-3. Time dependent of the degradation of MEF during the ozonation and O3/UV process at various pH values. (Experimental conditions:CMEF0: 0.5 mg L-1; and Ozone dose: 0.2 mg L-1). (a) pH 4, (b) pH 7, and (c) pH 9 4-19 Figure 4-2-4. Time dependent of the degradation of MEF during the ozonation and O3/UV process at various levels of pH value. (CMEF0: 0.5 mg L-1; and Ozone dose: 0.7 mg L-1) 4-20 Figure 4-2-5 Observed and calculated ozone degradation during (a) ozonation; (b) O3/UV processes of synthetic water (dotted lines are the calculated results). Systems: (Experimental conditions:CMEF0: 0.5 mg L-1, O3:0.2 mg L-1) 4-24 Figure 4-3-1 Effect of Humic acid on the degradation of MEF during (a) ozonation and (b) O3/UV process at various pH values 4-26 Figure 4-3-2 Effect of alkalinity on the degradation of MEF during (a) ozonation and (b) O3/UV process at various pH values 4-29 Figure 4-5-1 The formation of aldehyde for MEF at different levels of pH in the ozonation and O3/UV process. (Experimental condition:CMEF0: 0.5 mg L-1; and Ozone dose: 0.2 mg L-1) 4-33 Figure 4-6-1 The effect of ozone concentration and pH value on MEF degradation. (UV: 8 W; reaction time: 55 min; humic acid: 3 mg L-1; alkalinity: 35 mg L-1 as CaCO3) 4-41 Figure 4-6-2 The effect of UV light and reaction time value on MEF degradation. (O3: 0.2; pH: 4; humic acid: 3 mg L-1; alkalinity: 35 mg L-1 as CaCO3) 4-42 Figure 4-6-3 The effect of humic acid and alkalinity value on MEF degradation. (O3: 0.2; pH: 4; UV: 8 W; humic acid: 3 mg L-1) 4-43 List of Tables Table 2-2-1 Physical, chemical and pharmacological toxic properties of mefenamic acid 2-4 Table 2-2-2 Influent and effluent concentrations and removal efficiency of MEF in conventional sewage treatment plants in Europe 2-5 Table 2-3-1 Selected GC-MS analytical methods applied to the determination of pharmaceuticals in aqueous samples 2-7 Table 2-3-2 Selected Solid phase microextration (SPME) analytical methods applied to the determination of pharmaceuticals in aqueous sample 2-10 Table 2-3-3 Selected Derivatization-GC-MS analytical methods applied to the determination of pharmaceuticals in aqueous samples 2-12 Table 2-4-1 Treatment of pharmaceuticals in waters by AOPs 2-14 Table 3-3-1 GC/MS conditions for determining NASID compound 3-8 Table 4-1-1 Nitrate formation and TOC reduction by ozonation process and O3/UV process 4-10 Table 4-2-1 Results of regression of the developed model during ozonation process and O3/UV process 4-23 Table 4-3-1 UV254 and TOC reduction by ozonation and O3/UV processes 4-27 Table 4-4-1 Kinetic parameters obtained from experimental runs at different pH value on ozonation and O3/UV process. 4-31 Table 4-5-1 Ozonation by-products formation by ozonation 4-34 Table 4-5-2 Ozonation by-products yield coefficient (D) 4-36 Table 4-5-3 The carcinogenetic risk in different operational conditions 4-37 Table 4-6-1 ANOVA results of the quadratic model of MEF degradation 4-38 Table 4-6-2 Factors and levels in the six-factor three-level RSM design 4-39 | |
dc.language.iso | en | |
dc.title | 臭氧及臭氧/紫外光對Mefenamic acid去除影響之研究 | zh_TW |
dc.title | The Removal of Mefenamic acid from Water by Ozonation and O3 /UV | en |
dc.type | Thesis | |
dc.date.schoolyear | 98-2 | |
dc.description.degree | 碩士 | |
dc.contributor.coadvisor | 張怡怡 | |
dc.contributor.oralexamcommittee | 黃金寶,顧洋,曾迪華 | |
dc.subject.keyword | 甲芬納酸,雙酚胺衍生污染物,臭氧,臭氧/紫外光操作程序,臭氧副產物,最佳化, | zh_TW |
dc.subject.keyword | Mefenamic acid,Diphenylamine derivative pollutant,Ozonation,O3/UV process,Ozonation by-product,Optimization, | en |
dc.relation.page | 128 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2010-07-27 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 環境工程學研究所 | zh_TW |
顯示於系所單位: | 環境工程學研究所 |
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