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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 駱尚廉 | |
dc.contributor.author | Yi-Pei Chen | en |
dc.contributor.author | 陳沂珮 | zh_TW |
dc.date.accessioned | 2021-06-08T01:51:44Z | - |
dc.date.copyright | 2016-08-02 | |
dc.date.issued | 2016 | |
dc.date.submitted | 2016-07-25 | |
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Efficient electrochemical oxidation of perfluorooctanoate using a Ti/SnO2-Sb-Bi anode. Environmental Science & Technology, 45, 2973-2979. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/19277 | - |
dc.description.abstract | 全氟辛酸 (perfluorooctanoic acid, PFOA) 為環境中持久性新興污染物。其具有良好之穩定性及相容性、表面活性、低表面張力以及疏水、疏油性等特性,作為含氟表面活性劑廣泛應用於乳化劑、表面處理及防水材料。近年來,隨著 PFOA 使用量的增加,其廣泛分佈於全球環境系統中,因 PFOA 在環境介質中的穩定性、持久性和生物累積性所造成的污染問題備受關注。由於 PFOA 化學穩定性甚強,其於自然環境中不會降解,傳統之生物處理、氧化處理、Fenton 法、光解及光催化對其皆無良好之去除效率。
於簡易操作條件下,以檸檬酸鈦(III) 作為電子提供者之還原系統對 PFOA 之去除及礦化效率皆比過硫酸鹽之氧化系統佳,因氟原子之高電負性使其具有強烈接受電子的傾向,故還原途徑更利於 PFOA 礦化脫氟。結合奈米零價銅金屬與採用維生素 B12 作為吸附與催化劑促進還原系統硼氫化鈉、零價鐵及檸檬酸鈦(III) 對全氟辛酸進行還原降解,結果顯示,檸檬酸鈦(III) 對 PFOA 之還原脫氟效率高且穩定性佳,且將檸檬酸鈦(III) 結合維生素 B12與奈米零價銅金屬,於溶液初始 pH、檸檬酸鈦(III)、維生素 B12與奈米零價銅金屬分別為 9.0、45 mM、0.2 mM 及 2 g/L,於 70°C 之厭氧條件下,此簡易仿生系統可達到 65% 之 PFOA 去除率。 產物以 X 光繞射儀 (X-ray Diffractometer, XRD)、掃描電子顯微鏡 (Scanning Electron Microscope, SEM) 與X 射線光電子能譜儀 (X-ray Photoelectron Spectroscopy, XPS) 進行分析,檸檬酸鈦(III) 還原系統可直接脫除 α - position 之氟原子,產生氫取代全氟羧酸進一步降解,而 HPLC 無偵測出短鏈之全氟羧酸物質,以質量平衡與偵測氟離子之濃度符合 PFOA 之降解結果。 故於此低毒性、可生物降解性、仿生且對環境造成之衝擊度低檸檬酸鈦(III) 還原系統能夠提高全氟辛酸之可生物分解性,降低含 PFOA 廢水的生物毒性,反應機制主要為 PFOA 吸附於銅金屬表面後經由還原脫氟降解。 | zh_TW |
dc.description.abstract | Perfluorooctanoic acid (PFOA) has been considered as emerging persistent organic pollutants. It is a fluorosurfactant, widely used as emulsifying agents, surface treatment ingredients and water repellents due to its unique high stability, compatibility, high surface-active effect, low surface tension as well as both hydrophobic and oleophobic properties. In recent years, as the use of PFOA has increased, it is globally present in the environment. The stability, persistence and bioaccumulative properties of PFOA make it have an adverse effect on human health and ecosystem, and has drawn considerable interest from the public and regulatory agencies. It is thus crucial to evolve effective methods for the degradation of PFOA. This compound shows high chemical stabilization and it is not degraded in the natural environment or by conventional treatment methods, such as biology, ozonation, Fenton processes, photolysis, or photocatalysis. Using persulfate and Ti(III) citrate as reaction medium for oxidation and reduction degradation of PFOA, reductive defluorination of PFOA is more efficient than oxidative defluorination. Due to its strong electronegativity, the fluorine atom has high electron withdrawing capability, and acts as the reaction center. Thus, reductive defluorination of PFOA is more practical than oxidative defluorination. Catalyzed by vitamin B12 and copper nanoparticles was examined in batch systems using sodium borohydride, nano zero valent iron and titanium (III) citrate as the bulk reductant, a very efficient reduction for the conversion of PFOA to less-noxious compounds was achieved with Ti(III) citrate. A maximum removal was observed with an copper dose of 2 g L-1, Ti(III) citrate (45 mM), vitamin B12 (0.2 mM) at an initial pH of 9.0 and 70°C. In anoxic aqueous solution, the biomimetic reduction system was effectively removed 65% of PFOA. The products characterized by X-Ray diffraction (XRD), scanning electron microscopy (SEM) and X-ray Photoelectron Spectroscopy (XPS). The mass balance of fluoride matched the observed degradation of PFOA, while no short-chain perfluorocarboxylic acids byproducts were detected using HPLC. Consequently, highly efficient enhanced reduction systems were constructed for remediation of PFOA contaminated water. The removal of PFOA by TC/VB12/Cu can be attributed to the following main mechanisms: (i) adsorption onto copper surface and (ii) reduction via defluorination. | en |
dc.description.provenance | Made available in DSpace on 2021-06-08T01:51:44Z (GMT). No. of bitstreams: 1 ntu-105-R03541118-1.pdf: 3725221 bytes, checksum: 9269fa43d95c1860d3a61ac9fdfc9213 (MD5) Previous issue date: 2016 | en |
dc.description.tableofcontents | 口試委員審定書 ii
謝誌 iii 摘要 iv Abstract v 圖目錄 ix 表目錄 xii 第一章 緒論 1 1.1 研究緣起 1 1.2 研究目的 2 1.3 研究內容 3 第二章 文獻回顧 5 2.1 全氟和多氟烷基化合物 5 2.1.1 全氟和多氟烷基化合物之基本性質 5 2.1.2全氟和多氟烷基化合物之環境危害特性 6 2.1.3全氟和多氟烷基化合物毒理研究及其人體暴露途徑 10 2.1.4 環境中全氟和多氟烷基化合物污染之處理整治方法 10 2.1.5 全氟和多氟烷基化合物之污染現況 18 2.1.6 全氟和多氟烷基化合物之規範與管制 19 2.1.7 全氟辛酸之結構與物化特性 21 2.1.8 全氟辛酸之降解處理技術 23 2.2 檸檬酸鈦(III) 還原劑 24 2.3 電子媒介體 30 2.3.1 電子媒介體作用 30 2.3.2 維生素 B12 之特性與其反應原理 32 2.4 零價銅金屬與奈米化金屬顆粒 37 2.4.1 零價銅金屬性質 37 2.4.2 零價銅金屬的應用 39 2.4.3 奈米化金屬顆粒 41 第三章 研究方法 43 3.1 研究與實驗架構 43 3.2 實驗試劑與設備 45 3.2.1. 實驗使用試劑 45 3.2.2. 實驗使用設備 46 3.3 儲備溶液配製 46 3.3.1 全氟辛酸儲備溶液 46 3.3.2 維生素 B12 儲備溶液 46 3.4 零價金屬與分散劑的製備 46 3.4.1 配製零價銅金屬 46 3.4.2 還原劑的配製 47 3.4.3 批次實驗反應系統 47 3.5 污染物與衍生物濃度之分析儀器與方法 48 3.5.1 高效液相層析儀 (High-Performance Liquid Chromatography) 48 3.5.2 離子層析儀 (Ion Chromatograph) 49 3.6 反應系統濃度檢測機制分析之儀器與方法 50 3.6.1 檸檬酸鈦(III) 之檢測 50 3.6.2 維生素 B12 及其衍生物之檢測 51 3.6.3 紫外光�可見光分光光譜儀 (UV/VIS Spectrophotometer) 51 3.7 產物特性之分析儀器與方法 52 3.7.1 掃描電子顯微鏡 (Scanning Electron Microscope, SEM) 52 3.7.2 X 光繞射儀 (X-ray Diffractometer, XRD) 52 3.7.3 X 射線光電子能譜儀 (X-ray Photoelectron Spectroscopy, XPS) 54 3.7.4 傅立葉轉換紅外線光譜儀 (Fourier-Transform Infrared Spectrometer, FTIR) 55 第四章 結果與討論 57 4.1 背景實驗 57 4.1.1 反應容器之影響 57 4.1.2 檸檬酸鈦(III) 之環境參數影響 58 4.1.3 檸檬酸鈦(III) 於反應系統之氧化降解 59 4.1.4 全氟辛酸劑量 61 4.2 還原系統之選擇 63 4.2.1 還原劑選擇 63 4.2.2 硼氫化鈉與檸檬酸鈦(III) 之比較 68 4.2.3 零價鐵與檸檬酸鈦(III) 之比較 69 4.2.4 各還原劑之去除機制與效率比較 70 4.3 氧化與還原系統比較 71 4.4 檸檬酸鈦(III) 還原系統 74 4.4.1催化劑與厭氧條件於檸檬酸鈦(III) 系統之作用 74 4.4.2 檸檬酸鈦(III) 還原系統中各單元之作用 76 4.4.3 檸檬酸鈦(III) 之作用機制 80 4.4.4 維生素 B12 之作用機制 81 4.4.5 奈米零價銅金屬之作用機制 85 4.5 產物分析 90 4.5.1 SEM 分析奈米零價銅金屬反應前後之變化 90 4.5.2 XRD 分析晶體相位 92 4.5.2.1 奈米零價銅金屬反應前後之晶體相位 92 4.5.2.2 檸檬酸鈦(III) 反應後產物之晶體相位 94 4.5.3 FTIR 分析表面官能基特性 99 4.5.3.1 奈米零價銅金屬反應前後之表面官能基特性 99 4.5.3.2 檸檬酸鈦(III) 還原系統反應後產物之表面官能基特性 103 4.5.4 XPS 分析元素之價態 105 4.5.4.1 奈米零價銅金屬反應後之元素價態 106 4.5.4.2 檸檬酸鈦(III) 系統反應後之元素價態 107 4.6 機制探討 109 4.7 環境效益評估 113 第五章 結論與建議 115 5.1 結論 115 5.2 建議 116 參考文獻 118 | |
dc.language.iso | zh-TW | |
dc.title | 以維生素 B12 及零價銅金屬催化檸檬酸鈦(III) 進行全氟辛酸還原脫氟之應用 | zh_TW |
dc.title | Reductive Defluorination of Perfluorooctanoic Acid by Titanium(III) Citrate with Vitamin B12 and Copper Nanoparticles. | en |
dc.type | Thesis | |
dc.date.schoolyear | 104-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 林進榮,胡景堯 | |
dc.subject.keyword | 催化脫氟,奈米零價銅,全氟辛酸,還原,維生素 B12, | zh_TW |
dc.subject.keyword | Catalytic defluorination,Copper nanoparticles,Perfluorooctanoic acid,Reductive,Vitamin B12, | en |
dc.relation.page | 131 | |
dc.identifier.doi | 10.6342/NTU201601100 | |
dc.rights.note | 未授權 | |
dc.date.accepted | 2016-07-25 | |
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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