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研究生:陳俊銘
研究生(外文):Chun-ming Chen
論文名稱:受戴奧辛污染之環境介質經Fenton處理之研究
論文名稱(外文):Study of the Fenton Process on the Treatment of Dioxins-contaminated Enviromental Media
指導教授:許皓捷許皓捷引用關係
指導教授(外文):Hau-Jie Shiu
學位類別:碩士
校院名稱:國立臺南大學
系所名稱:環境生態研究所碩士班
學門:環境保護學門
學類:環境資源學類
論文種類:學術論文
畢業學年度:96
語文別:中文
論文頁數:76
中文關鍵詞:Fenton飛灰土壤底泥同分異構物戴奧辛
外文關鍵詞:DioxinsFentonFly ashsoilsedimentisomer
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過去針對環境介質之戴奧辛去除係以熱處理技術為主,但熱處理技術耗損能量且成本昂貴,本研究以Fenton處理受戴奧辛污染之環境介質,Fenton處理屬高級氧化程序之一環,透過添加雙氧水及亞鐵產生氫氧自由基(OH•)進行環境介質中戴奧辛之異相催化氧化。前人研究指出Fenton法去除戴奧辛有不錯的成效,但僅限於模擬樣本,對於環境介質之樣本是否實際具可行性,值得進一步探討。
本研究進行三種不同環境介質(處理廠飛灰、土壤及底泥)之基本特性分析,先進行阿太堡試驗並以統一土壤分類法 (USCS)進行土壤判定,結果顯示處理廠飛灰屬低壓縮性的砂質無機性黏土(CL),而土壤與底泥則屬於低至中壓縮性的有機質粉土 (OL);經XRF及XRD分析判斷處理廠飛灰主要晶相為NaCl,而土壤與底泥則為SiO2;經由TGA分析發現本研究採樣之環境介質在25~900℃間有一明顯的熱重損失(Weight Loss),顯示本研究採樣之處理廠飛灰、土壤與底泥等環境介質含有機物,且經由高解析氣象層析儀/質譜儀(HRGC/MS)分析後發現本研究採樣之環境介質已超法規標準判屬戴奧辛有害事業廢棄物。
本研究將受戴奧辛污染之環境介質經Fenton處理後進行固液相分析,當Fenton處理之雙氧水添加劑量越高,固相戴奧辛與液相有機物之處理效果越佳;本研究分別以100~550、550~900及100~900℃之熱重損失探討環境介質中固相有機物與戴奧辛毒性當量之相關性,研究結果顯示處理廠飛灰與底泥於100~900℃之熱重損失與其戴奧辛毒性當量相關性較佳,土壤則以100~550℃之熱重損失與其戴奧辛毒性當量(TEQ)相關性較佳;就戴奧辛毒性當量貢獻而言, 1,2,3,7,8-PeCDD、2,3,7,8-TeCDD、1,2,3,7,8-PeCDF及2,3,4,6,7,8-HxCDF為貢獻處理廠飛灰戴奧辛毒性當量之主要物種,而1,2,3,4,6,7,8-HpCDD、OCDD、1,2,3,4,6,7,8-HpCDF及OCDF則為貢獻土壤及底泥戴奧辛毒性當量之主要物種,經本研究發現受戴奧辛污染之環境介質經Fenton處理後,因受本身有機物之影響導致戴奧辛之特徵圖譜並無明顯差異。
In the past, dioxins-contaminated environmental media were mostly treated by thermal process which has been considered energy-consumable and costly. The aim of this study is to discuss the treatment of dioxins-contaminated environmental media by Fenton process. Fenton process is one method involved in advanced oxidation processes (AOPs). Due to the addition of hydrogen peroxide and ferrous ions, OH free radical (OH•) is able to attack dioxins-contaminated environmental media by heterogeneous catalytic oxidation. Although previous studies has pointed out that Fenton processes is possible to treat dioxins with high removal efficiency, However, only simulated media were discussed in these studies. Thus, the feasibility of Fenton process on the treatment of actual dioxins-contaminated environmental media is worthwhile.
In this study, primary characteristics of environment media such as fly ash sampled from waste treatment plant, soil and sediment sampled from contaminated site were discussed. Base on the results of Atterberg experiment, fly ash is classified as CL (low compressibility sandy inorganic clay); soil and sediment are classified as OL (to lower to compressibility organic matter silty soil) by unified soil classification system (USCS). Base on the analysis of X-ray fluorescence (XRF) and X-ray diffractomer (XRD), it shows that the main crystalline phase of fly ash is NaCl, and the main crystalline phase of soil and sediment is SiO2. Base on the analysis of thermogravimetry analysis (TGA), weight loss in the range from 25 to 900℃ is obviously, which means that organic content was involved in these environmental media. Toxic equivalent (TEQ) of dioxin for these environmental media is analyzed by HRGC/MS (High Resolution Gas Chromatograph/Mass Spectrometer), it shows that these environment media sampled are above the regulation standard, which are classified as dioxin-hazardous waste.
The analysis of liquid and solid phase for three dioxins-contaminated environmental media after Fenton process was done in this study. It shows that as the dosage of hydrogen peroxide for Fenton Process is increased, the removal efficiency of dioxin in solid phase is increased. By the way, the removal efficiency of organics in liquid phase is also increased. In order to discuss the relationships between dioxin and organic content in solid phase of dioxins-contaminated environmental media after Fenton process, weight loss of 100~550, 550~900 and 100~900℃ were evaluated as organic content in solid phase of these environmental media by furnace. It reveals that weight loss of 100~900℃ for fly ash and sediment has higher relativity to TEQ of dioxin. However, weight loss of 100~550℃ for soil has higher relativity to TEQ of dioxin. As to the contributions of TEQ for each dioxin isomers from these environment media, 1,2,3,7,8-PeCDD, 2,3,7,8-TeCDD, 1,2,3,7,8-PeCDF and 2,3,4,6,7,8-HxCDF are major dioxin species in fly ash. Furthermore, 1,2,3,4,6,7,8-HpCDD, OCDD, 1,2,3,4,6,7,8-HpCDF and OCDF are major dioxin isomers in soil and sediment. Apparently, the specific profiles of dioxin in these environment media after Fenton process are not changed apparently for high organic content involved.
摘要 I
Abstract III
致謝 V
總目錄 VII
表目錄 X
圖目錄 XI
符號表 XII
第一章 緒論 1
1-1 研究緣起 1
1-2 研究目的 2
第二章 文獻回顧 3
2-1何謂戴奧辛 3
2-1-1 戴奧辛來源 4
2-1-2 戴奧辛之毒性及危害 6
2-2 戴奧辛於環境介質中之流佈 8
2-2-1 戴奧辛之傳輸 8
2-2-2 土壤的吸持 8
2-2-3 環境介質與有機物之關係 9
2-3 受戴奧辛污染之環境介質 10
2-3-1 飛灰中之戴奧辛之特徵 11
2-3-2 土壤與底泥中之戴奧辛之特徵 13
2-3-3 環境介質中戴奧辛整治方法 15
2-4 Fenton處理技術 19
2-4-1 Fenton法原理 19
2-4-2 Fenton法反應機制 20
2-4-3 Fenton法反應條件 21
2-4-4 Fenton法對環境介質中戴奧辛之處理 22
第三章� 實驗方法與步驟 23
3-1 實驗流程 23
3-2 採樣地點 24
3-2-1 採樣區 24
3-3 樣本採樣方法 24
3-3-1 土壤採樣 24
3-3-2 底泥採樣 24
3-3-3 處理廠飛灰採樣 25
3-4 試驗設備 25
3-5分析方法 26
3-5-1 阿太堡試驗 27
3-5-2 XRF分析 28
3-5-3 XRD分析 28
3-5-4 COD分析 28
3-5-5 TGA分析 29
3-5-6 有機物分析 29
3-5-7 戴奧辛檢測分析 29
3-5-8 資料分析方法 35
第四章� 結果與討論 36
4-1 環境介質之基本特性 36
4-1-1 阿太堡試驗 36
4-1-2 環境介質之XRF及XRD分析 38
4-1-3 環境介質之TGA分析 41
4-1-4 環境介質之COD分析 43
4-1-5 環境介質之戴奧辛分析 44
4-2 環境介質經Fenton處理後固液相有機物之探討 45
4-2-1 環境介質經Fenton處理後之戴奧辛 45
4-2-2 環境介質經Fenton處理後之液相有機物分析 48
4-2-3 環境介質經Fenton處理後之固相有機物分析 50
4-2-4 環境介質有機物與戴奧辛之關係 52
4-3 環境介質經Fenton處理後戴奧辛同分異構物之探討 55
4-3-1 受戴奧辛污染環境介質經Fenton處理異構物個別濃度之分析 55
4-3-2 受戴奧辛污染環境介質經Fenton處理異構物毒性當量之分析 61
第五章� 結論與建議 68
5-1 結論 68
5-2 建議 69
參考文獻 70
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