指導教授:駱尚廉臺灣大學:環境工程學研究所郭子寧Kuo, Tzu-NingTzu-NingKuo2014-11-302018-06-282014-11-302018-06-282014http://ntur.lib.ntu.edu.tw//handle/246246/264170This study was focused on PFOA decomposition in persulfate solution catalyzed iron-modified activated carbon. to by Fe/AC to decompose PFOA. With the process impregnation and calcination, the redox state Fe covered on AC can promote the generation of sulfate radicals and the elevation of decomposition of PFOA. In order to explore the different factors influence the performance, experiments were designed for the effect of pesulfate dosage, Fe/AC dose, Fe covered ratio, pH, temperature, ferrous ion and the radical inhibitors. The decomposition and defluorination efficiency of PFOA were higher in Fe/AC-PS system than that of PS system. Moreover, the PFOA removals increased with the increasing PS dosage. For the experiments of Fe/AC dose and Fe covered ratio, results indicated that the decomposition and defluorination efficiency of PFOA improved with the promotion of Fe/AC dose and Fe ratio but decreased if the amounts were excess. Under neutral condition, PFOA decomposition efficiency was better than that in acidic condition because too much sulfate radicals produced would hinder the oxidation, and the worst in base conditions due to the suppression by OH-. Compared the efficiency of catalysis by Fe2+ and Fe/AC, experiments results illustrated that Fe/AC is more effective based on the function of catalysis as well as adsorption. The tert-Butanol served as the radical inhibitor that result in the decline of the decomposition and defluorination efficiency of PFOA. It proved that tert-Butanol can scavenge the sulfate radicals.口試委員審定書 i 誌謝 ii 摘要 iii Abstract iv 目錄 v 圖目錄 ix 表目錄 xi 第一章 緒論 1 1.1前言 1 1.2研究目的 2 1.3研究內容 4 第二章 文獻回顧 5 2.1 PFCs危害性與污染特性 5 2.1.1 PFCs之基本性質 5 2.1.2 PFOA之化合物特性 6 2.1.3 PFOA之產源及環境宿命 8 2.1.4 PFOA對人體和生物體影響 10 2.1.5 國內PFOA與PFOS管制狀況 11 2.2 PFCs之處理技術 12 2.2.1高溫燃燒法 12 2.2.2高級氧化法 12 2.2.3光化學氧化法 14 2.2.4超音波化學氧化法 15 2.2.5活性碳吸附法 16 2.3過硫酸鹽氧化劑 18 2.3.1過硫酸鹽種類與ISCO使用 19 2.3.2過硫酸鹽溶解於水中反應 20 2.3.3其它催化過硫酸鹽之方法 22 2.3.4過硫酸鹽實際應用 23 2.4活性碳吸附理論及催化氧化劑機制和應用 26 2.4.1活性碳吸附理論 26 2.4.2活性碳等溫吸附模式 26 2.4.3活性碳吸附動力模式 27 2.4.4活性碳改質 29 2.4.5活性碳催化氧化劑機制及實際應用 30 第三章 實驗方法與材料 33 3.1研究架構 33 3.2實驗試劑 35 3.3鐵改質活性碳製備 36 3.4實驗分析方法 36 3.4.1高效液相層析儀 36 3.4.2離子層析儀 38 3.4.3場發射掃描式電子顯微鏡 39 3.4.4比表面積與孔徑分析儀 39 3.4.5 XRD粉末繞射分析儀 41 3.5 PFOA降解實驗步驟 41 3.6 PFOA降解實驗操作參數 42 3.6.1過硫酸鹽濃度影響試驗 42 3.6.2鐵改質活性碳劑量影響試驗 42 3.6.3鐵披覆活性碳比例影響試驗 42 3.6.4 pH值影響試驗 43 3.6.5溫度影響試驗 43 3.6.6亞鐵離子催化與Fe/AC催化影響比較 43 3.6.7自由基抑制劑影響試驗 43 第四章 結果與討論 44 4.1背景實驗 44 4.2鐵改質活性碳特性分析 46 4.2.1掃描式電子顯微鏡分析 46 4.2.2 XRD粉末繞射、BET與界達電位探討 52 4.3過硫酸鹽濃度效應 54 4.3.1過硫酸鹽系統 54 4.3.2鐵改質活性碳結合過硫酸鹽系統 55 4.4鐵改質活性碳添加劑量效應 63 4.5鐵披覆活性碳比例效應 70 4.6 pH及溫度效應 73 4.6.1 pH效應 73 4.6.2溫度效應 76 4.7亞鐵離子催化結合系統降解效應比較 78 4.8自由基抑制劑對PFOA降解影響 80 4.9 結合系統機制探討 83 4.9.1 PFOA礦化機制 83 4.9.2降解系統機制 84 第五章 結論與建議 85 5.1結論 85 5.2建議 86 參考文獻 87 附錄 983464308 bytesapplication/pdf論文使用權限:不同意授權全氟辛酸過硫酸鹽鐵改質活性碳催化亞鐵離子以鐵改質活性碳結合過硫酸鹽系統降解全氟辛酸之研究Decompositions of PFOA in Persulfate solution catalyzed by Iron-Modified Activated Carbonthesishttp://ntur.lib.ntu.edu.tw/bitstream/246246/264170/1/ntu-103-R01541113-1.pdf