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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 駱?廉 | |
dc.contributor.author | Yu-Chieh Chou | en |
dc.contributor.author | 周宥節 | zh_TW |
dc.date.accessioned | 2021-06-16T08:43:01Z | - |
dc.date.available | 2013-09-02 | |
dc.date.copyright | 2013-09-02 | |
dc.date.issued | 2013 | |
dc.date.submitted | 2013-08-24 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/58989 | - |
dc.description.abstract | 本研究係以微波氧化程序(MOP)來進行掩埋場滲出水之研究,主要探討的因子有酸鹼值、溫度、氧化劑濃度、微波功率及微波照射時間。研究中以熱效應、過硫酸鹽氧化、微波照射之總有機碳移除量來探討MOP的微波特殊效應(Microwave - Specific effects),實驗結果發現MOP相較於傳統加熱氧化(CHO)效果提升10%,除了在微波低功率(128W/85℃/1M Na2S2O8 和128W/85℃/2M Na2S2O8) 效果不如CHO外,其餘MOP大多呈現加乘效果,且隨著溫度上升,加乘效果更明顯,這是因為MOP與CHO加熱機制不同的緣故。在整個加熱過程,不論是MOP或CHO過程,過硫酸根離子皆呈現快速的消耗,並轉換成硫酸根離子,造成其殘留之過硫酸根離子濃度不足,難以持續降解TOC及COD。本研究也針對MOP及CHO過程,其有機酸的生成降解曲線進行探討,並著重於MOP之衍生有機酸生成機制。實驗結果表示,草酸的生成降解曲線在MOP及CHO過程非常類似,由25℃上升至85℃過程,滲出水中之草酸皆因過硫酸鹽的熱催化產生的氧化作用而降解;草酸於10至70分鐘期間,因部分有機物降解生成新草酸;該草酸又於70至130分鐘期間,再度因微波氧化而持續降解,隨後,草酸曲線因殘留氧化力不足呈現草酸濃度停滯情形。觀測MOP及CHO實驗過程,該酸鹼值因衍生有機酸的生成分別下降了0.51及0.65 pH單位,於MOP實驗中,草酸是主要的有機酸衍生物,依實驗結果推斷,乳酸的生成似由蘋果酸的降解;草酸則由草酸前驅物質或其他有機酸降解而成;醋酸於MOP過程,呈現快速降解及快速生成的特性,為一種短暫存留的中間型產物;乳酸在過硫酸鹽濃度過低(952 mg/L)或過高(4762 mg/L)劑量下,僅生成少量或無乳酸形成,於本研究,僅在適當過硫酸鹽濃度2381 mg/L,方能利於乳酸的累積。本研究最後也針對MOP的可行性及成本進行分析,結果顯示MOP 550W/85℃/1M在5分鐘內可完成80%到90%色度移除率;30分鐘內可完成80%到90% TOC移除率;30分鐘內可完成65%到70% UV254移除率;40分鐘內可完成45%到55% COD移除率。在相同的加溫時間下,MOP成本約為181 NTD/m3 ,略低於CHO為183 NTD/m3。此外,MOP不用調整處理水的酸鹼值,所以可省下pH值控制的成本,經評估MOP具有成為前處理程序之潛力。 | zh_TW |
dc.description.abstract | Microwave oxidation process (MOP) was evaluated for treatment of landfill leachate. The experimental parameters include pH, temperature, oxidant doses, microwave power setting, and irradiation time. The study explored the microwave-specific effects of the MOP. The contributions of pure thermal, persulfate oxidation and microwave irradiation on TOC removal were quantified. It was then found the combinations of them were usually synergistic in MOP except two of them were antagonistic (128W/85℃/1M Na2S2O8 and 128W/85℃/2M Na2S2O8) due to the difference in the heating mechanisms between conventional heating oxidation (CHO) and MOP. At the highest temperature tested (85℃) in this study, microwave irradiation may cause generation and termination of oxidizing radicals at adverse rates. The study also found that persulfate decayed rapidly in either MOP or CHO treatment of landfill leachate. Besides, this study compared formation and degradation behaviors of organic acids in landfill leachate under MOP and CHO and explored derivative mechanisms of organic acids in MOP. The results showed that formation and degradation behaviors of oxalic acid (OA) were very similar under CHO and MOP, in which its concentrations decreased in the temperature-raising period, then increased due to decomposition of TOC from 10 to 70 min, decreased due to persulfate oxidation from 70 to 130 min, and stayed the same afterwards. The pH values of the leachate solution dropped 0.51 and 0.65 pH units after MOP and CHO treatment, respectively. OA was the dominant organic acid formed in MOP. The derivative mechanisms of organic acids were developed using the experimental results. Lactic acid (LA) was generated from decomposition of malic acid (MA), and OA was formed from oxidation of its precursors. Acetic acid (AA) was formed and soon decomposed. LA had its maximum concentration with a persulfate dose of 2381 mg/L, while lower or higher persulfate doses yielded few or no LA in MOP. The study also evaluated the feasibility of MOP and the cost, the results showed MOP 550W/85℃/1M had color removals of 80% to 90% within 5 minutes, TOC removals of 70% to 80% within 30 minutes, UV254 removals of 65% to 70% within 30 minutes, and COD removals of 45% to 55% within 40 minutes. Within the same heating time, electric cost of MOP (181 NTD/m3) was slightly lower than that of CHO (183 NTD/m3). Besides, MOP was suit to use in wide pH range and more cost saving without pH-controlled, so MOP was an alternative of pre-treatment. | en |
dc.description.provenance | Made available in DSpace on 2021-06-16T08:43:01Z (GMT). No. of bitstreams: 1 ntu-102-D96541002-1.pdf: 1239086 bytes, checksum: 7bcd146e3e833250b4772666a2a2bacc (MD5) Previous issue date: 2013 | en |
dc.description.tableofcontents | Content
謝誌 I 中摘 III Abstract V Content VII Lists of Figures X List of Tables XVII 1. Introduction 1 1.1 Research Motivation 1 1.2 Research Objectives 2 1.3 Research Content 3 2. Literature Review 5 2.1 Landfill Leachate 5 2.2 Microwave Technique and Principle 6 2.3 Microwave Oxidation -Persulfate 9 2.4 Microwave irradiation versus Conventional Heating 12 2.5 Characteristics of the Organic Acids in AOPs 14 3. Research Method 18 3.1 Characteristics of the landfill leachate 18 3.2 Materials 20 3.3 Experimental Apparatus 21 3.4 Experimental Procedure 23 4. Results and Discussion 27 4.1 Effects of Persulfate Oxidation 27 4.1.1 Persulfate Oxidation at 25℃ 27 4.1.2 Persulfate Oxidation at 55℃ 32 4.1.3 Persulfate Oxidation at 85℃ 37 4.2 Effects of Microwave Irradiation 41 4.2.1 Microwave irradiation versus TOC concentration 41 4.2.2 MW versus pH 43 4.2.3 Effects of UV254 and Color removals on MW 47 4.3 Effects of Microwave Oxidation Process 52 4.3.1 Calorimetric equation 52 4.3.2 Effects of Persulfate Doses, Microwave Power Settings and pH 54 4.3.3 Discussion on Microwave-Specific Effects 65 4.4 MOP versus CHO 74 4.5 Formation and degradation of oxalic acids 79 4.6 Formation and degradation mechanisms of derivative organic acid 92 4.7 Assess the Feasibility of MOP to Treat Landfill Leachates 110 5. Conclusions 118 5.1 The Microwave Oxidation of Landfill Leachate 118 5.2 Formation and Degradation Mechanisms of Organic Acids 118 5.3 Assess the Feasibility of MOP to be Pre-Treatment 120 5.4 Further Suggestions 120 References 122 Appendix 138 Lists of Figures Figure 1-1 Research Framework 4 Figure 3-1 Extended Aeration Method in Sanjuku Landfill. 18 Figure 3-2 The characteristics of raw leachate from 01/2008 to 01/2012 (Data were from the Sanjuku Landfill). 20 Figure 3-3 The microwave reactor of Milestone Terminal 320 (Milestone, Ethos Touch Control, USA). 22 Figure 3-4 The Average Column Retention time of each organic acid. 25 Figure 4-1 TOC concentrations versus persulfate doses at 25℃ (Na2S2O8 doses = 4762 and 9524 mg/L; initial pH of the leachate =7.02; temperature = 25℃ and reaction time = 130 minutes). 28 Figure 4-2 Kinetic analysis of TOC concentration versus time without presence of persulfate at 25℃ (leachate = 50 mL; initial pH of the leachate =7.02; temperature = 25℃ and reaction time = 130 minutes). 29 Figure 4-3 Kinetic analysis of TOC concentrations versus time in persulfate oxidation at 25℃ (Na2S2O8 doses = 4762 mg/L; initial pH of the leachate =7.02; temperature = 25℃ and reaction time = 130 minutes). 30 Figure 4-4 Kinetic analysis of TOC concentrations versus time in persulfate oxidation at 25℃ (Na2S2O8 doses = 9524 mg/L; initial pH of the leachate =7.02; temperature = 25℃ and reaction time = 130 minutes). 31 Figure 4-5 TOC concentrations versus persulfate doses at 55℃ (Na2S2O8 doses = 4762 and 9524 mg/L; initial pH of the leachate =7.02; temperature = 55℃ and reaction time = 130 minutes). 33 Figure 4-6 Kinetic analysis of TOC concentration versus time without presence of persulfate at 55℃ (leachate = 50 mL; initial pH of the leachate =7.02; temperature = 55℃ and reaction time = 130 minutes). 34 Figure 4-7 Kinetic analysis of TOC concentrations versus time in persulfate oxidation at 55℃ (Na2S2O8 doses = 4762 mg/L; initial pH of the leachate =7.02; temperature = 55℃ and reaction time = 130 minutes). 35 Figure 4-8 Kinetic analysis of TOC concentrations versus time in persulfate oxidation at 55℃ (Na2S2O8 doses = 9524 mg/L; initial pH of the leachate =7.02; temperature = 55℃ and reaction time = 130 minutes). 36 Figure 4-9 TOC concentrations versus persulfate doses at 85℃ (Na2S2O8 doses = 4762 and 9524 mg/L; initial pH of the leachate =7.02; temperature = 85℃ and reaction time = 130 minutes). 37 Figure 4-10 Kinetic analysis of TOC concentration versus time without presence of persulfate at 85℃ (leachate = 50 mL; initial pH of the leachate =7.02; temperature = 85℃ and reaction time = 130 minutes). 38 Figure 4-11 Kinetic analysis of TOC concentrations versus time in persulfate oxidation at 85℃ (Na2S2O8 doses = 4762 mg/L; initial pH of the leachate =7.02; temperature = 85℃ and reaction time = 130 minutes). 39 Figure 4-12 Kinetic analysis of TOC concentrations versus time in persulfate oxidation at 85℃ (Na2S2O8 doses = 9524mg/L; initial pH of the leachate =7.02; temperature = 85℃ and reaction time = 130 minutes). 40 Figure 4-13 TOC concentrations versus Temperature and microwave irradiation time (microwave power = 128W and 550W; temperature = 25, 55, and 85℃). 42 Figure 4-14 TOC concentrations versus pH and microwave irradiation time (microwave power = 550W; temperature = 85℃; initial pH of leachate: 3, 5, 7, and 9). 44 Figure 4-15 COD concentrations versus pH and microwave irradiation time (microwave power = 550W; temperature = 85℃; initial pH of leachate: 3, 4, 5, 7, and 9). 45 Figure 4-16 COD concentrations versus time: (a) MW, and (b) CH (temperature = 85℃; microwave power = 550W; initial pH of leachate: 7.04). 46 Figure 4-17 UV254 versus Temperature and microwave irradiation time (microwave power = 128W and 550W; temperature = 25, 55, and 85℃; initial pH of leachate: 7.04). 49 Figure 4-18 UV254 versus pH and microwave irradiation time (microwave power = 550W; temperature = 85℃). 50 Figure 4-19 Color versus Temperature and microwave irradiation time (microwave power = 128W and 550W; temperature = 25, 55, and 85℃; initial pH of leachate: 7.04). 51 Figure 4-20 TOC concentrations versus microwave power settings (Na2S2O8 doses = 952, 2381, and 4762 mg/L; initial pH of the leachate =7.04; temperature = 85℃ and irradiation time = 15 minutes). 54 Figure 4-21 Persulfate concentrations as a function of microwave power setting and irradiation time (deionized water: 0.2M Na2S2O8 = 50 mL:1 mL; temperature = 85℃; Na2S2O8 doses =952 mg/L). 56 Figure 4-22 Persulfate concentrations as a function of microwave power setting and irradiation time (deionized water:0.5M Na2S2O8 = 50 mL:1 mL; temperature = 85℃; Na2S2O8 doses =2381 mg/L). 57 Figure 4-23 Persulfate concentrations as a function of microwave power setting and irradiation time (deionized water:1M Na2S2O8 = 50 mL:1 mL; temperature = 85℃; Na2S2O8 doses =4762 mg/L). 58 Figure 4-24 kinetic analysis of persulfate residuals versus microwave power settings: (a) 128W, (b) 325W, (c) 550W, and (d) 775W. 62 Figure 4-25 Color, UV254 and TOC removals versus microwave power setting (leachate:1M Na2S2O8 = 50 mL:1 mL; Na2S2O8 doses = 4762 mg/L; temperature = 85℃; initial pH of the leachate = 7.04; and irradiation time = 15 min). 63 Figure 4-26 TOC concentrations as a function of pH and microwave irradiation time (microwave power = 550W; temperature = 85℃; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 64 Figure 4-27 COD concentrations versus time in the microwave oxidation process (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 75 Figure 4-28 COD concentrations versus time in conventional heating oxidation (temperature = 85℃; initial pH of the leachate = 7; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 76 Figure 4-29 COD and persulfate concentrations versus reaction time (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.04; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 78 Figure 4-30 Formation and degradation of oxalic acid (a) MOP, and (b) MW. (microwave power = 550W; temperature = 85℃; initial pH of the leachate: (a) 6.96, (b) 7.13; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 82 Figure 4-31 Formation and degradation of oxalic acid: (a) CHO, and (b) CH (temperature = 85℃; initial pH of the leachate: (a) 7.12, (b) 7.15; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 84 Figure 4-32 Variations of solution pH and oxalic acid concentrations versus time: (a) MOP, (b) MW, (c) CHO, and (d) CH. 86 Figure 4-33 Use 3rd order polynomial regression to predict the maximum amounts of oxalic acids in MOP. 87 Figure 4-34 Use 2nd order polynomial regression to predict the maximum amounts of oxalic acids in MOP. 89 Figure 4-35 Use 3rd order polynomial regression to predict the maximum amounts of oxalic acids in CHO. 90 Figure 4-36 Use 2nd order polynomial regression to predict the maximum amounts of oxalic acids in CHO. 91 Figure 4-37 Formation and loss of organic acids during MOP treatment at pH 7 (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.1; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 95 Figure 4-38 The pathway of derivative organic acids (dashed line respected the minor reaction). 96 Figure 4-39 Concentrations of derivative organic acids under microwave irradiation with various persulfate doses (a) 0 mg/L (Raw leachate) (b) 952 mg/L (c) 2381 mg/L (d) 4762 mg/L (microwave power = 550W; temperature = 85℃; initial TOC of leachate = 473.5 mg/L; and initial pH of the leachate = 7.04). 97 Figure 4-40 Formation and loss of organic acids under acidic pH (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 5.02; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 104 Figure 4-41 Formation and loss of organic acids under neutral pH (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.01; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 105 Figure 4-42 Formation and loss of organic acids under alkaline pH (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 9.02; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 106 Figure 4-43 Formation and loss of organic acids under low persulfate doses (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.01; leachate:0.2M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 952 mg/L). 107 Figure 4-44 Formation and loss of organic acids under meddle persulfate doses (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.01; leachate:0.5M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 2381 mg/L). 108 Figure 4-45 The influence of pH in organic acids (a) Oxalic acid (b) Acetic acid (c) Lactic acid (d) Malic acid. (microwave power = 550W; temperature = 85℃; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 109 Figure 4-46 Comparison of TOC, Color, UV254 removals on MOP. (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.01; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 110 Figure 4-47 The correlation of UV254 and TOC in MOP (microwave power = 550W; temperature = 85℃; initial pH of the leachate = 7.01; leachate:1M Na2S2O8 = 50 mL:1 mL; and Na2S2O8 doses = 4762 mg/L). 111 List of Tables Table 2-1 The dielectric loss tangents of 25, 55, and 85℃. 8 Table 2-2 The reaction rates at mesophilic to high temperature. 11 Table 2-3 Microwave heating versus Conventional heating. 12 Table 2-4 Rearrangements of microwave treatments. 13 Table 2-5 Microwave application in environmental field. 16 Table 2-5 Microwave application in environmental field (Continuous). 17 Table 3-1 The concentrations of organic acids and humid acids of leachate. 25 Table 3-2 Characteristics of raw leachate. 26 Table 4-1 Time required to achieve the target temperature as a function of the microwave power. 53 Table 4-2 Contribution of persulfate doses and microwave power settings on pseudo first-order kinetics reaction rate. 59 Table 4-3 Microwave-Specific Effects on TOC removals. 72 Table 4-4 Contribution of pure thermal, microwave irradiation and persulfate on TOC reductions. 73 Table 4-5 Assess the parameters of MOP to treatment landfill leachate 116 Table 4-6 TOC removal rates of MOP versus persulfate doses and microwave power settings 117 | |
dc.language.iso | en | |
dc.title | 以微波氧化程序降解掩埋場滲出水有機物之研究 | zh_TW |
dc.title | The study of using microwave oxidation process to decompose organic substance of landfill leachate | en |
dc.type | Thesis | |
dc.date.schoolyear | 101-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 楊萬發,呂鴻光,高思懷,陳孝行,林正芳 | |
dc.subject.keyword | 滲出水,微波氧化,過硫酸鹽,傳統加熱,草酸,乳酸,醋酸, | zh_TW |
dc.subject.keyword | leachate,microwave oxidation,persulfate,conventional heating,oxalic acid,lactic acid,acetic acid, | en |
dc.relation.page | 163 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2013-08-27 | |
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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