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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 張慶源(Ching-Yuan Chang) | |
dc.contributor.author | Chia-Chi Chang | en |
dc.contributor.author | 張家驥 | zh_TW |
dc.date.accessioned | 2021-06-15T04:19:51Z | - |
dc.date.available | 2011-12-29 | |
dc.date.copyright | 2009-12-29 | |
dc.date.issued | 2009 | |
dc.date.submitted | 2009-10-29 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/45432 | - |
dc.description.abstract | 本研究使用高重力旋轉填充床(high-gravity rotating packed bed, HGRPB)做為氣-液接觸裝置提臭氧之氣-液質量傳送效率對水中溶解性有機物進行臭氧化反應。氣-液質量傳送效率為決定臭氧化系統氧化效率之主要限制因子。HGRPB相較於傳統之氣-質量傳送裝置其質量傳送效率較高。本研究並利用其高混合效率之特性,填入鉑觸媒(Pt/γ-Al2O3)做為觸媒接觸床以催化臭氧自解產生更高氧化能力之氫氧自由基,以提升系統整體氧化效能。系統分為旋轉填充床及光化學反應槽兩部分,以半批次式(semi-batch type)操作 ,並以酚(phenol)為測試物種進行HGRPB之操作測試,求取最適化之系統操作條件。其後,進一步針對生物難分解之環境賀爾蒙物種鄰苯二甲酸二甲酯(dimethyl phthalate, DMP)以臭氧相關之高級氧化程序(advanced oxidation processes, AOPs)加以處理,探討DMP之高級氧化之反應性與處理效果並建立其臭氧化分解反應機制。本研究以高重力臭氧化(high-gravity ozonation, HG-OZ)程序為基礎搭配觸媒及紫外光進行有機物高重力催化臭氧化分解,所比較程序包含高重力臭氧化反應(HG-OZ)、高重力觸媒催化臭氧化(HG catalytic OZ, HG-Pt-OZ)、高重力光催化臭氧化(HG photolysis OZ, HG-UV-OZ) 及高重力觸媒光催化臭氧化(HG-UV-Pt-OZ)。
研究結果顯示HGRPB達高重力狀態轉速(rotating speed, Nr)須在600 rpm (23.76 G)以上。臭氧之氣-液質量傳送係數(kLa)隨Nr增加而提昇。當Nr = 1,200 rpm時,其kLa = 0.0148 s-1。DMP之對臭氧之反應性雖然較phenol差,但以HG-OZ處理DMP在DMP初始濃度(CDMP0)為100 mg L-1、反應液體體積(VL)為1L、Nr為1,200 rpm及臭氧添加劑量(ozone applied dosage, mA,in)為1,500 mg L-1-sample時亦可將DMP完全分解。以HG-OZ處理DMP時可得Nr與DMP相對於mA,in之降解反應速率常數(kDMP)之關係為kDMP = 2 ×10-6 Nr + 0.0005。在HG-OZ處理DMP之系統中,於中性(以緩衝鹽控制pH = 7)時,其降解反應最為迅速,kDMP = 0.0042 (mg l-1)-1;然其總有機物(total organic carbon, TOC)分解則在鹼性(以緩衝鹽控制pH= 10)時礦化分解速率最為迅速,其kTOC = 0.0004 (mg l-1)-1。於HGRPB填充Pt/γ-Al2O3觸媒之HG-Pt-OZ系統,其DMP降解可進一步提升,pH = 7時其kDMP = 0.0067 (mg l-1)-1。而合併使用UV-C光源進行照射之HG-UV-Pt-OZ系統,可進一步分解水中殘留之溶解性臭氧形成氫氧自由基加速水中DMP及TOC分解。DMP之臭氧化降解以phthalate acid (PA)為主要中間產物,進一步臭氧化分解形成mucomic acid、glyoxalic acid、glyoxal、及formic acid等副產物。 | zh_TW |
dc.description.abstract | In this study, a high-gravity rotating packed bed (HGRPB) was used as a gas-liquid mass transfer equipment as well as ozonation reactor to decompose persistent organic pollutants (POPs). Ozonation is limited by its selective reactivity and gas-liquid mass transfer rate while HGRPB is an effective gas-liquid mixing equipment can increasing ozone mass transfer coefficient. The system consists of photoreactor and HGRPB and was carried out via semi-batch type operation. The platinum-containing catalyst (Pt/γ-Al2O3) packed in the HGRPB in conjunction with ozonation (HG-Pt-OZ) can enhance the self-decomposition of molecular ozone in liquid to form high reactive radical species and promote the oxidation ability of ozone in HG-OZ system. Phenol was firstly used to simulate the organic pollutant in HG-OZ based advanced oxidation processes (AOPs) to realize the operation characteristics of the HG system. Then the ozonation efficiency and mechanism of dimethyl phthalate (DMP) were further stuided. Different combinations of HG-OZ with Pt/γ-Al2O3 and UV for the degradation of DMP were tested. These include HG-OZ, HG catalytic OZ (HG-Pt-OZ), HG photolysis OZ (HG-UV-OZ) and HG-UV-Pt-OZ. The O3 gas-liquid mass transfer in HGRPB was also discussed in this study.
The results indicate that the rotating speed (Nr) needs to be higher than 600 rpm (23.76 G) for reaching the well high-gravity condition. The gas-liquid mass transfer coefficient (kLa) increases with Nr for which kLa = 0.0148 s-1 at Nr = 1,200 rpm. The resistance for ozonation of DMP is higher than that of phenol. However it is decomposed completely in all HG-OZ based AOPs at ozone applied dosage (mA,in) of 1,500 mg L-1-sample (with the conditions: intial concentration of DMP CDMP0 = 100 mg L-1, volume of liquid sample VL = 1 L, Nr = 1,200 rpm). The correlation relationship of Nr and DMP decomposition rate (kDMP) is kDMP = 2 ×10-6 Nr + 0.0005. In neutral condition (pH = 7), DMP has the best decomposition rate with kDMP = 0.0042 (mg l-1)-1. However, the total organic carbon has the signest mineralization rate in alkaline solution (pH = 10) with kTOC = 0.0004 (mg l-1)-1. The combined use of Pt/γ-Al2O3 in HG-OZ process (HG-Pt-OZ) can promote the decomposition of DMP with kDMP = 0.0067 (mg l-1)-1 at pH = 7. The UV-C irradiation in photoreactor can further decompose the residual dissolved ozone to form hydroxyl radicals to reduce DMP and TOC. Phthalate acid (PA) is the main intermediate in the beginning of DMP ozonation and further decomposed into mucomic acid, glyoxalic acid, glyoxal and formic acids in the course of ozonation. | en |
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dc.description.tableofcontents | 目 錄
中文摘要 i 英文摘要 iii 目錄 v 圖目錄 ix 表目錄 xiii 符號說明 xiv 第一章 緒 論 1 1.1 研究背景 1 1.2 研究目的 4 1.3 研究內容 5 第二章 文獻回顧 7 2.1臭氧之基本性質與反應機制 7 2.1.1臭氧的物理、化學性質 7 2.1.2臭氧在水中之自解反應 10 2.1.3 臭氧與有機物的反應 13 2.1.3.1臭氧與有機物的反應行為特性 13 2.1.3.2 pH值對臭氧與有機物之反應行為特性的影響 16 2.2 高級氧化之原理與反應機制 18 2.2.1自由基特性 18 2.2.2苯環上的親電子取代反應 20 2.3臭氧觸媒催化反應 22 2.3.1 同相催化反應 24 2.3.2 異相催化反應 25 2.4超重力旋轉填充床之原理及應用 32 2.4.1.高重力工程技術之發展 32 2.4.2高重力旋轉填充床氣液接觸器之構造與原理 36 2.4.3 高重力旋轉填充床氣液接觸器之特性及其應用 38 2.4.3.1壓降之影響 38 2.4.3.2溢流現象 38 2.4.3.3液膜質量傳送係數 38 2.4.3.4氣膜質量傳送係數 39 2.4.4 高重力旋轉填充床氣液接觸器之應用 40 2.5 鄰苯二甲酸二甲酸酯類 43 2.5.1鄰苯二甲酸酯類之來源與應用 43 2.5.2 鄰苯二甲酸酯類之特性與環境流布 45 2.5.3 鄰苯二甲酸酯類之主要分解作用 48 2.5.4 鄰苯二甲酸二甲酯相關處理文獻 49 第三章 實驗方法 51 3.1 實驗材料與設備 51 3.2臭氧高重力旋轉填充床反應系統特性實驗 58 3.1.1高重力臭氧反應槽之設計、裝置及預備實驗 58 3.2.2系統基礎水力測試 61 3.3 HGRPB之操作特性與觸媒催化分解酚實驗 63 3.4高重力氧化程序運用於環境賀爾蒙之處理 65 第四章 結果與討論 69 4.1高重力系統基礎測試 69 4.2.1 水力停留時間測試 69 4.1.2 填充床不同轉速下之氣-液質傳 75 4.2 HGRPB之操作特性與觸媒催化實驗 80 4.2.1. 不同填充材料之吸附實驗 81 4.2.2 phenol之高重力臭氧化反應 83 4.2.3 phenol之高重力臭氧催化實驗 88 4.2.3.1 不同種類觸媒之影響 88 4.2.4 UV光照射對高重力臭氧化之影響 93 4.2.5 UV光照射對phenol之高重力臭氧催化氧化之影響 96 4.2.6 高重力臭氧化反應綜合討論 100 4.3鄰苯二甲酸二甲酯之高重力催化臭氧化分解 104 4.3.1 DMP之臭氧化分解 104 4.3.2 DMP之高重力臭氧化分解反應 106 4.3.3 操作模式之影響 109 4.3.4 Nr對臭氧化之影響 112 4.3.5 pH值之影響 116 4.3.6 UV光照射對DMP之高重力臭氧氧化之影響 124 4.3.7 DMP高重力臭氧觸媒催化分解 136 4.4 DMP臭氧化分解反應機制之探討 155 第五章 結論與建議 161 5.1 結論 161 5.2 建議 163 參考文獻 164 附錄 A觸媒催化臭氧化基礎反應條件測試 172 A-1臭氧反應中觸媒粒徑之影響 174 A-2 CSTR系統中UV之影響 176 B 酚及鄰苯二甲酸二甲酯之觸媒催化分解實驗 180 圖 目 錄 Fig. 1-1 The framework of the research. 6 Fig. 2-1 The mechanism of gaseous ozone generation 8 Fig. 2-2 The extreme forms of resonance structures in ozone molecules 8 Fig. 2-3 Reaction diagram for ozone decomposition process. 13 Fig. 2-4 Reaction mechanism of ozone with organic in water. 14 Fig. 2-5 Ozone decomposition process in water. 17 Fig. 2-6 Schematic of ozonation of o-cresol. 21 Fig. 2-7 Proposed mechanism for oxalic acid catalytic ozonation by means of the Co(II)/O3system. 25 Fig. 2-8 The concept of ozonation combined with adsorption. 29 Fig. 2-9 Scheme illustrating the possible mechanism for ozonation process in the presence of metal-support (metal oxide) catalyst 30 Fig.2-10 Description of HGRPB. 35 Fig. 2-11 Cross-flow RPB. 35 Fig. 2-12. Adsorption and transport modes of PAEs. 48 Fig. 2-13. Hydrolysis of DMP at various pH value. 50 Fig. 3-1 Flow chart for the study. 57 Fig. 3-2 Type I HG system 59 Fig. 3-3 Type II HG system 60 Fig. 4-1 Hydrolytic retention time vs. rotating speed of HGRPB. 70 Fig. 4-2 HRT vs. liquid flow rate of HGRPB. 71 Fig. 4-3 Gas and liquid distribution at low Nr in HGRPB. 74 Fig. 4-4 Variations of dissolved ozone concentration via different Nr in HGRPB. 76 Fig. 4-5 Variations of Ln[CDO3*/(C DO3*-C DO3)] via different Nr in HGRPB. 78 Fig. 4-6 Variations of KLa with Nr in HGRPB. 79 Fig. 4-7 Adsorption of aqueous phenol on Pt/γ-Al2O3 in HGRPB systems of HG and HG-Pt. 82 Fig. 4-8 Variations of Cphe/Cphe0 with mA,in in HG-OZ process. 85 Fig. 4-9 Variations of CTOC/CTOC0 with time for the mineralization of phenol via ozonation and photolysis ozonation in HGRPB. 86 Fig. 4-10 The relationships of ηTOC, ηphe and pH value with mA,in. 87 Fig. 4-11 The conventionally proposed scheme of oxidation of phenol in aqueous solution by ozone or hydroxyl radical 87 Fig. 4-12 Variation of Cphe/Cphe0 with mA,in for HG-Cat-OZ process at various ms of Pt/γ-Al2O3 89 Fig. 4-13 Variations of CTOC/CTOC0 with mA,in for the mineralization of phenol via HG-Cat-OZ processes. 90 Fig. 4-14 Variations of CTOC/CTOC0 with mA,in for the mineralization of phenol via HG-Cat-OZ processes. 91 Fig. 4-15 Variations of CTOC/CTOC0 with time for the mineralization of phenol via ozonation and photolysis ozonation in HGRPB. 94 Fig. 4-16 Ozone absorption spectrum 95 Fig. 4-17 Variations of ηTOC with mA,in for the mineralization of phenol using different ozone-assisted AOPs in HGRPB. 98 Fig. 4-18 The relationships of ηTOC, ηphe and pH value with mA,in in HG-Pt-UV-OZ system. 99 Fig. 4-19 Plots of natural logarithm of the relative organic concentration vs. time for different HG systems. 102 Fig. 4-20 Simplified scheme illustrating the possible mechanism for the ozonation of phenol with UV and catalyst 103 Fig. 4-21 The molecular structure of DMP 104 Fig. 4-22 Variations of CDMP/CDMP0 during ozonation and OZ-UV process of DMP in CSTR 105 Fig. 4-23 Time variations of CDMP/CDMP0 for the decomposition of DMP in HG systems. 108 Fig. 4-24 Variations of CDMP/CDMP0 of DMP with mA,in in different HG operation type. 110 Fig. 4-25 Variations of TOC/TOC0 of DMP with mA,in in different HG operation type. 111 Fig. 4-26 Effects of mA,in on the decomposition of DMP for the HG-OZ process at various Nr. 113 Fig. 4-27 Plots of natural logarithm of the relative organic concentration vs. mA,in for for the HG-OZ process at various Nr. 114 Fig. 4-28 The relationship of kDMP, Nr and KLa for the HG-OZ processes. 115 Fig. 4-29 Effects of pH value on the decomposition of DMP for the HG-OZ process 118 Fig. 4-30 Effects of pH value on the decomposition of TOC for the HG-OZ process. 119 Fig. 4-31 Plots of natural logarithm of CDMP/CDMP0 vs. mA,in for various pH values in the HG-OZ processes. 120 Fig. 4-32 Plots of natural logarithm of TOC concentration vs. mA,in for various pH values in the HG-OZ processes. 120 Fig. 4-33 Variation of dissolved O3 concentration (CDO3) in HG-OZ processes for different pH value. 123 Fig. 4-34 DMP absorption spectrum. 125 Fig. 4-35 Emission spectrum of UV lamp 126 Fig. 4-36 Time variations of CDMP/CDMP0 for the decomposition of DMP in HG-UV 127 Fig. 4-37 The variations of CDMP/CDMP0 for the decomposition of DMP in HG-UV 128 Fig. 4-38 The variations of CDMP/CDMP0 for the decomposition of DMP in HG-OZ and HG-UV-OZ processes. 130 Fig. 4-39 The variations of TOC/TOC0 for the decomposition of DMP in HG-OZ and HG-UV-OZ processes. 131 Fig. 4-40 Absorption spectrum of DMP. 134 Fig. 4-41 The UV transmittance of DMP, dissolved O3 and H2O. 135 Fig. 4-42 CDMP/CDMP0 vs. mA,in during ozonation of DMP in HGRPB. 138 Fig. 4-43 Mechanisms of DMP catalytic ozonation via Pt/γ-Al2O3. 139 Fig. 4-44 Variations of pH value during ozonation of DMP in HGRPB. 141 Fig. 4-45 CDMP/CDMP0 vs. mA,in in various pH value of DMP in HG-Pt-OZ system. 142 Fig. 4-46. TOC/TOCC0 vs. mA,in in various pH value of DMP in HG-Pt-OZ system. 143 Fig. 4-47 The variation of CDO3 with mA,in in various pH value of DMP in HG-Pt-OZ system. 145 Fig. 4-48 CDMP/CDMP0 vs. time during ozonation of DMP for HG-UV-Pt. 147 Fig. 4-49 TOC/TOC0 vs. time during ozonation of DMP for HG-UV-Pt. 148 Fig. 4-50 CDMP/CDMP0 vs. mA,in during ozonation of DMP in HGRPB. 151 Fig. 4-51 CDMP/CDMP0 vs. mA,in during ozonation of DMP in HGRPB for various pH value. 152 Fig. 4-52 TOC/TOC0 vs. mA,in during ozonation of DMP in HGRPB for various pH value. 153 Fig. 4-53 The variation of CDO3 with mA,in in various pH value of DMP in HG-UV-Pt-OZ system. 154 Fig. 4-54 Simplified scheme illustrating the possible mechanism for the ozonation of DMP with UV and catalyst. 156 Fig. 4-55 The electrophilic attack of DMP via ozonation 157 Fig. 4-56 The decyclization of PA via ozonation 158 Fig. 4-57 The identification of DMP ozonation intermediates. 159 Fig. 4-58 Schematic of ozonation of DMP. 166 Fig. A-1. CSTR system 173 Fig. A-2 Variations of TOC/TOC0 of catalytic ozonation in CSTR. 175 Fig. A-3 Variations of TOC/TOC0 of catalytic ozonation in CSTR. 177 Fig. A-4 Variations of pH value during ozonation phenol in CSTR. 178 Fig. A-5 Variations of ORP value of ozonation in CSTR. 179 Fig. B-1 Variations of C/C0 during ozonation of DMP and phenol in HGRPB for HG-UV-Pt-OZ. 182 Fig. B-2 Variations of pH value during ozonation of DMP and phenol in HGRPB for HG-UV-Pt-OZ. 183 表 目 錄 Table 2-1 The physical and chemical properties of gaseous ozone 9 Table 2-2 The reduction potentials of various oxidants 10 Table 2-3 Solubility of ozone and air in water 10 Table 2-4 Half-life time of ozone in water 11 Table 2-5 Radical types of different AOPs 20 Table 2-6 Two mechanisms for the catalytic decomposition of aqueous ozone. 28 Table 2-7 Average rates of the decomposition of aqueous ozone on metal catalysts 31 Table 2-8 Comparison of conventional packed bed and high-gravity rotating packed bed gas-liquid contactors 37 Table 2-9 Physicochemical characteristics of dimethyl phthalate 47 Table 3-1 Physical characteristics of DASH-220N 64 Table 4-1 Theoretical value of Rt and t with various QLR 73 Table 4-2. The gas-liquid mass transfer coefficient of O3 and G force at various Nr in HG system 77 Table 4-3. Pseudo-first order kinetic rate constants of decomposition of TOC for different HG processes 101 Table 4-4. The ηDMP via various working gases 107 Table 4-5. The k DMP value of DMP in HG-OZ reaction for various Nr 114 Table 4-6. The kDMP and kTOC value of DMP in HG-OZ reaction for various pH value 117 Table 4-7 The irradiation intensity of the UV lamp 132 Table 4-8 The kDMP and kTOC value of DMP in HG-UV-OZ reaction for various pH value 133 Table 4-9 The kDMP and kTOC value of DMP in HG-OZ reaction for various pH value 144 Table 4-10 The kDMP and kTOC value of DMP in HG-UV-Pt-OZ reaction for various pH value 156 Table 4-11. The main intermediates of DMP ozonation at different reaction stage 160 | |
dc.language.iso | zh-TW | |
dc.title | 應用高重力旋轉填充床反應器於觸媒臭氧處理程序以去除水中之鄰苯二甲酸二甲酯 | zh_TW |
dc.title | Application of High-gravity Rotating Packed Bed for Catalytic Ozonation of Dimethyl Phthalate in Aqueous Solution | en |
dc.type | Thesis | |
dc.date.schoolyear | 98-1 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 蔣本基,李俊福,張添晉,陳孝行 | |
dc.subject.keyword | 臭氧,臭氧催化,觸媒,旋轉填充床,酚,鄰苯二甲酸二甲酯, | zh_TW |
dc.subject.keyword | Ozonation,catalytic ozonation,catalyst,high-gravity rotating packed bed (HGRPB),phenol,dimethyl phthalate (DMP), | en |
dc.relation.page | 183 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2009-10-29 | |
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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