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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/81297完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 駱尚廉(Shang-Lien Lo) | |
| dc.contributor.author | Yuan-Han Liu | en |
| dc.contributor.author | 劉元涵 | zh_TW |
| dc.date.accessioned | 2022-11-24T03:41:33Z | - |
| dc.date.available | 2021-08-06 | |
| dc.date.available | 2022-11-24T03:41:33Z | - |
| dc.date.copyright | 2021-08-06 | |
| dc.date.issued | 2021 | |
| dc.date.submitted | 2021-07-23 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/81297 | - |
| dc.description.abstract | "全氟化物為良好的介面活性劑，具有熱穩定性和化學穩定性之化學特性，並常被用於工業產品中，許多文獻證實長碳鏈全氟化物全氟辛酸 (Perfluorooctanoic acid, PFOA) 與全氟辛烷磺酸 (Perfluorooctanesulfonic acid, PFOS)對環境與人體具有危害性，已被許多國家限制使用，故轉而使用短碳鏈全氟丁烷磺酸(Perfluorobutanesulfonic Acid, PFBS)，作為長碳鏈全氟化物的替代化學品，現今許多環境水體中已測出PFBS，因此開發有效的PFBS處理方法勢在必行。 本研究利用UV/亞硫酸鹽系統光催化誘發水合電子，以還原降解PFBS，並探討不同實驗參數對UV/亞硫酸鹽系統降解PFBS之影響。由結果顯示，濃度20.0 mg/L PFBS溶液之最佳降解參數為亞硫酸鹽濃度0.02M，初始pH值為11，系統溫度45℃，攪拌速率300rpm，於系統反應360分鐘後，可達到去除率79.2 %、脫氟率58.3 %，且生成短鏈全氟羧酸和氟離子，而PFBS去除之反應速率常數為0.33 hr-1，脫氟之反應速率常數為0.21 hr-1。PFBS處理效能與初始pH值和反應溫度呈正相關，曝氮氣呈負相關，而系統中亞硫酸鹽濃度過高，會抑制PFBS之處理效能。由中間產物分析結果表明，水合電子還原降解PFBS主要有三種降解途徑分別為脫磺酸反應、H/F交換反應以及C–C的斷鍵反應。 本研究以最佳參數降解PFOA與PFOS，利用反應動力學比較PFBS、PFOA與PFOS三者，其結果顯示擬一階降解的反應速率常數PFOA > PFOS > PFBS，而降解之反應活化能(Ea)分別為90.2 kJ/mole、319.4 kJ/mole與364.6 kJ/mole。PFBS、PFOA與PFOS三者之去除與脫氟的反應速率會與官能基、氟烷基鏈長度與C–F鍵低鍵離解能的位置和數量有關。同時本研究開發二階反應模型，可準確預測UV/亞硫酸鹽系統在15℃ ~ 45℃之溫度範圍下，PFBS、PFOA與PFOS於各反應時間下之去除率與脫氟率。" | zh_TW |
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| dc.description.tableofcontents | 口試委員會審定書 i 致謝 ii 摘要 iii Abstract iv 目錄 vi 圖目錄 ix 表目錄 xi 第一章 前言 1 1.1研究緣起 1 1.2研究目的 2 1.3研究內容 2 第二章 文獻回顧 4 2.1全氟化物 4 2.1.1全氟化物之污染來源與環境危害 4 2.1.2短碳鏈全氟化物使用現況 5 2.1.3短碳鏈全氟化物特性與環境分布 5 2.2全氟化物之處理方法 8 2.2.1活性碳吸附法 8 2.2.2濾膜法 9 2.2.3直接光解與光催化氧化法 9 2.2.4電化學氧化法 10 2.2.5超聲波氧化法 10 2.3 高級還原處理法—UV/亞硫酸鹽還原方法 12 2.3.1 UV/亞硫酸鹽系統 12 2.3.2 UV/亞硫酸鹽生系統水合電子生成反應 14 2.3.3初始pH值對降解全氟化物之影響 15 2.3.4亞硫酸鹽濃度對全氟化物降解之影響 15 2.3.5水中溶氧對全氟化物降解之影響 16 2.3.6溫度濃度對全氟化物降解之影響 17 2.3.7反應動力學探討 17 2.3.8全氟羧酸化合物之降解機制 20 2.3.9全氟磺酸化合物之降解機制 22 第三章 材料與方法 24 3.1 研究內容與架構 24 3.2 實驗試劑與設備 26 3.2.1 實驗試劑 26 3.2.2 實驗設備 28 3.3分析方法 30 3.4實驗操作與參數設定 39 3.4.1背景實驗 39 3.4.2最佳參數實驗 40 3.4.3反應動力學實驗 41 3.5品質管制 42 第四章 結果與討論 43 4.1背景實驗 43 4.1.1反應槽吸附實驗 43 4.1.2控制實驗—紫外光光解實驗 43 4.1.3控制實驗—亞硫酸鹽 45 4.2最佳參數實驗 49 4.2.1初始pH值對UV/亞硫酸鹽系統去除PFBS的影響 49 4.2.2亞硫酸鹽濃度對UV/亞硫酸鹽系統去除PFBS的影響 51 4.2.3曝氮氣對UV/亞硫酸鹽系統去除PFBS的影響 53 4.3 UV/亞硫酸鹽系統反應動力學探討 55 4.3.1溫度對UV/亞硫酸鹽系統去除PFBS的影響 55 4.3.2溫度對UV/亞硫酸鹽系統去除PFOA與PFOS的影響 57 4.3.3擬一階反應動力學模型 60 4.3.4二階反應動力學模型 66 4.4 UV/亞硫酸鹽系統降解之中間產物 74 4.4.1降解PFBS中間產物分析結果 74 4.4.2降解PFOA中間產物分析結果 79 4.4.3降解PFOS中間產物分析結果 81 4.5 UV/亞硫酸鹽系統降解PFBS機制 83 4.6 UV/亞硫酸鹽系統pH值分析結果 86 4.7 EPR自由基鑑定結果 88 第五章 結論與建議 91 5.1結論 91 5.2建議 92 參考資料 93 附錄 100 | |
| dc.language.iso | zh-TW | |
| dc.subject | 全氟辛酸 | zh_TW |
| dc.subject | 全氟丁烷磺酸 | zh_TW |
| dc.subject | 水合電子 | zh_TW |
| dc.subject | UV/亞硫酸鹽 | zh_TW |
| dc.subject | 全氟辛烷磺酸 | zh_TW |
| dc.subject | hydrated electron | en |
| dc.subject | Perfluorobutanesulfonic acid (PFBS) | en |
| dc.subject | Perfluorooctane sulfonate (PFOS) | en |
| dc.subject | Perfluorooctanoic acid (PFOA) | en |
| dc.subject | UV/sulfite | en |
| dc.title | 以UV/亞硫酸鹽光催化還原全氟丁烷磺酸之研究 | zh_TW |
| dc.title | The Study of UV/Sulfite Photo-reduction of Perfluorobutanesulfonic Acid | en |
| dc.date.schoolyear | 109-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 郭繼汾(Hsin-Tsai Liu),胡景堯(Chih-Yang Tseng) | |
| dc.subject.keyword | 全氟丁烷磺酸,全氟辛烷磺酸,全氟辛酸,UV/亞硫酸鹽,水合電子, | zh_TW |
| dc.subject.keyword | Perfluorobutanesulfonic acid (PFBS),Perfluorooctane sulfonate (PFOS),Perfluorooctanoic acid (PFOA),UV/sulfite,hydrated electron, | en |
| dc.relation.page | 125 | |
| dc.identifier.doi | 10.6342/NTU202101658 | |
| dc.rights.note | 同意授權(限校園內公開) | |
| dc.date.accepted | 2021-07-23 | |
| 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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