請用此 Handle URI 來引用此文件：
http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/42611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 | Yi-Ling Wu | en |
| dc.contributor.author | 吳憶伶 | zh_TW |
| dc.date.accessioned | 2021-06-15T01:17:40Z | - |
| dc.date.available | 2014-07-28 | |
| dc.date.copyright | 2009-07-28 | |
| dc.date.issued | 2009 | |
| dc.date.submitted | 2009-07-27 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/42611 | - |
| dc.description.abstract | 本研究以濕式氧化法(wet air oxidation, WAO)及催化濕式氧化法(catalytic WAO, CWAO)處理甲基丙烯酸甲酯(methyl methacrylate, MMA)。於CWAO中，使用自製磁性鉑觸媒(Pt/ZrO2/SiO2/Fe3O4, Pt/ZSM)進行MMA之催化氧化分解並與商用鉑觸媒Pt/γ-Al2O3之催化氧化效能進行比較。研究結果顯示WAO對MMA降解率(ηMMA)及化學需氧量(chemical oxygen demand, COD)礦化率(ηCOD)主要受溫度影響。反應溫度(TST)越高，MMA降解效果越顯著。於WAO中，當TST = 493 K，pO2 = 1.63 MPa (於參考溫度Trf = 493 K時，氧之分壓)，及MMA初始濃度CMMA0 = 500 mg L-1，反應三小時後，ηMMA及ηCOD分別為87％及30％。
超順磁性鉑觸媒Pt/ZSM為次微米顆粒(100~200 nm)，飽合磁化量為6.54 emu g-1，且具有高比表面積(67.46 m2 g-1)及高鉑含量(13.37 wt.% Pt)。其界達電位值(pHZPC)為4.7，故可有效吸附MMA經氧化反應後之中間產物有機酸，並可維持觸媒的催化效能。以添加六氯鉑酸(H2PtCl6．6H2O)之含浸法製備時，水熱還原法可將鉑完全還原；而氣態還原法之Pt以PtCl62-形式存在於表面，殘留的氯離子會影響催化反應。 以氧氣為工作氣體控制反應條件為TST = 453 K，pO2 = 1 MPa (Trf = 453 K)及觸媒添加量(mS) = 1 g時進行CWAO處理MMA及COD，氣態還原法觸媒HG-Pt/ZSM (ηMMA及ηCOD分別為29％及54％) 及水熱還原法觸媒HT-Pt/ZSM (ηMMA及ηCOD分別為46％及36％)之反應性與商用鉑觸媒Pt/γ-Al2O3 (ηMMA及ηCOD分別為39％及39％)相當。反應後之Pt/ZSM觸媒依舊具有超順磁性特性(6.5-7.3 emu g-1)，故應用高梯度磁性分離機(high-gradient magnetic separation, HGMS)分離後，可將觸媒回收再利用，此為Pt/ZSM在固相分離時優於Pt/γ-Al2O3之處。 | zh_TW |
| dc.description.abstract | This study investigated the treatment of methyl methacrylate (MMA) via wet air oxidation (WAO) and catalytic wet air oxidation (CWAO) processes. A superparamagnetic platinum catalyst (Pt/ZrO2/SiO2/Fe3O4, Pt/ZSM) was used to promote the decomposition of MMA and compared with commercial platinum catalyst Pt/γ-Al2O3. Effects of major operating parameters on the system performances in terms of normalized concentrations of MMA and chemical oxygen demand (COD) were investigated. The operating parameters examined included the setting temperature (TST), partial pressure of O2 (pO2), initial concentration of MMA (CMMA0), amount of catalyst used (mS) and reaction time (t). The decomposition efficiencies of MMA and COD (ηMMA and ηCOD) can respectively reach 87 and 30％ after 3 hr reaction time via WAO with reaction conditions at TST = 493 K, pO2 = 2.18 MPa (expressed as value at reference temperature Trf of 493 K) and CMMA0 = 500 mg L-1.
The Pt/ZSM exhibits particle size of around 100-200 nm, magnetization of 6.54 emu g-1, specific external surface area of 67.46 m2 g-1, and with high platinum content of 13.37 wt.%. The pHZPC of Pt/ZSM is 4.7 which is favorable for the effective adsorption of acid intermediates on the catalyst surface. The hydrothermal method can reduce the chloride content of the Pt/ZSM which is prepared by the impregnation of Pt precursor H2PtCl6．6H2O on the support of ZSM. At TST = 453 K, pO2 = 1 MPa (Trf = 453 K), and mS = 1 g, the reactivities of HG-Pt/ZSM (Pt/ZSM with Pt reduced via H2 gas) (ηMMA = 29％ and ηCOD = 54％) and HT-Pt/ZSM (Pt/ZSM with Pt reduced via hydrothermal method) (ηMMA = 46％ and ηCOD = 36％) to decompose MMA and COD are as good as those of Pt/γ-Al2O3 (ηMMA = 39％ and ηCOD = 39％). The Pt/ZSM catalyst still holds superparamagnetic property with saturation magnetization of 6.5-7.3 emu g-1 after being used in CWAO process. Thus the used Pt/ZSM can be separated via high-gradient magnetic separation (HGMS) fot the reuse. | en |
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| dc.description.tableofcontents | 致謝 i
中文摘要 ii Abstract iii 目錄 v 圖目錄 viii 表目錄 xviii 符號說明 xix 第一章 緒論 1 1.1研究背景 1 1.2研究內容 2 1.3研究目的 3 第二章 文獻回顧 5 2.1磁性材料 5 2.1.1磁性的種類 5 2.1.2超順磁性(Superparamagnetic) 12 2.1.3鐵氧化物 13 2.2高梯度磁性分離機 16 2.2.1高梯度磁性分離機原理 16 2.2.2高梯度磁性分離機相關文獻 17 2.3磁性觸媒製備法 18 2.3.1化學共沉澱法(Coprecipitation) 18 2.3.2溶膠凝膠法 19 2.3.3含浸法(Impregnation) 26 2.3.4水熱法(Hydrothermal) 26 2.4濕式氧化法 28 2.4.1濕式氧化法原理 28 2.4.2濕式氧化法反應機制 30 2.4.3濕式氧化反應動力學 31 2.4.4濕式氧化反影響因素 32 2.4.5觸媒催化濕式氧化 33 2.5甲基丙烯酸甲酯 37 2.5.1甲基丙烯酸甲酯之來源 37 2.5.2甲基丙烯酸甲酯之特性 37 2.5.3甲基丙烯酸甲酯之相關處理文獻 39 第三章 實驗設備與研究方法 40 3.1 實驗藥品與材料 40 3.2設備 42 3.2.1磁性吸附劑之合成設備 42 3.2.2磁性分離機設備 42 3.2.3濕式氧化設備 42 3.2.4分析儀器設備 43 3.3實驗架構與進行步驟 44 3.3.1觸媒之製備 44 3.3.2磁性鉑觸媒之物理化學特性鑑定 48 3.3.3濕式氧化反應 49 3.3.4磁性分離機特性試驗 54 第四章 結果與討論 56 4.1超順磁性鉑觸媒之基本性質 56 4.1.1表面電位 56 4.1.2顆粒型態 60 4.1.3比表面積 63 4.1.4元素半定性分析 64 4.1.5顆粒磁滯曲線 68 4.1.6 XRD 70 4.1.7磁性鉑觸媒清洗步驟之氯離子濃度變化 73 4.2濕式氧化反應分解MMA 74 4.2.1 MMA濕式氧化分解機制之探討 74 4.2.2升溫程序對MMA分解之影響 75 4.2.3工作氣體種類之影響 79 4.2.4反應溫度之影響 79 4.2.5反應壓力之影響 83 4.2.6甲基丙烯酸甲酯初始濃度之影響 87 4.3觸媒濕式催化(CWAO)分解MMA 89 4.3.1 Pt/γ-Al2O3 89 4.3.2 Pt/ZSM 120 4.3.3 綜合比較 141 4.3.4濕式氧化後氯離子釋出試驗 146 4.3.5濕式氧化後回收之Pt/ZSM觸媒 147 4.3.6濕式氧化後觸媒之磁滯曲線 147 4.3.7濕式氧化後觸媒之XRD 150 4.3.8觸媒溶出試驗 158 4.4磁性分離機特性試驗 159 4.4.1進流水濃度影響 159 4.4.2進流水流速影響 161 第五章 結論與建議 164 5.1結論 164 5.1.1磁性鉑觸媒之物理化學特性 164 5.1.2濕式氧化程序 164 5.1.3 Pt/γ-Al2O3濕式催化氧化程序 165 5.1.4 Pt/ZSM濕式催化氧化程序 165 5.2建議 166 參考文獻 167 附錄A. EDX之半定性分析 a 附錄B. 觸媒溶出試驗ICP-OES e 附錄C. WAO反應溫度及壓力 l 附錄D. MMA之檢量線 w 附錄E. 實驗數據 y | |
| dc.language.iso | zh-TW | |
| dc.subject | 甲基丙烯酸甲酯 | zh_TW |
| dc.subject | 濕式氧化 | zh_TW |
| dc.subject | 濕式催化分解 | zh_TW |
| dc.subject | 鉑觸媒 | zh_TW |
| dc.subject | 超順磁性 | zh_TW |
| dc.subject | 水熱還原法 | zh_TW |
| dc.subject | reductive hydrothermal method | en |
| dc.subject | methyl methacrylate | en |
| dc.subject | Wet air oxidation (WAO) | en |
| dc.subject | catalytic wet air oxidation (CWAO) | en |
| dc.subject | Pt catalyst | en |
| dc.subject | superparamagnetic | en |
| dc.title | 磁性觸媒應用於催化濕式氧化程序處理水中溶解性污染物之研究 | zh_TW |
| dc.title | Application of Magnetic Catalyst for Catalytic Wet Air Oxidation of Organics in Aqueous Solution | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 97-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 張瓊芬(Chiung-Fen Chang),張奉文(Feg-Wen Chang) | |
| dc.subject.keyword | 濕式氧化,濕式催化分解,鉑觸媒,超順磁性,水熱還原法,甲基丙烯酸甲酯, | zh_TW |
| dc.subject.keyword | Wet air oxidation (WAO),catalytic wet air oxidation (CWAO),Pt catalyst,superparamagnetic,reductive hydrothermal method,methyl methacrylate, | en |
| dc.relation.page | 173 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2009-07-28 | |
| 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 | |
文件中的檔案：
| 檔案 | 大小 | 格式 | |
|---|---|---|---|
| ntu-98-1.pdf 未授權公開取用 | 2.75 MB | Adobe PDF |
系統中的文件，除了特別指名其著作權條款之外，均受到著作權保護，並且保留所有的權利。