以熱裂解去除土壤中六氯苯之效率探討

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林信賢(Hsin-hsien Lin) 查詢紙本館藏

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論文名稱

以熱裂解去除土壤中六氯苯之效率探討
(Removal of hexachlorobenzene from soil by pyrolysis)

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摘要(中)

六氯苯過去廣泛應用於農業作為制菌劑，具有難降解、生物累積毒性等特性，為疏水性物質，易和土壤行疏水性吸附而難以去除。本研究配置六氯苯污染土壤，以靜態及動態熱裂解兩種方式，分別探討土壤中六氯苯去除效率及氯苯分布，並嘗試添加零價鐵，探討其在熱裂解系統中對六氯苯去除效率之影響。靜態結果顯示未添加零價鐵，操作時間60分鐘，250oC、300oC、350oC及400oC之六氯苯去除效率為18%、42%、74%及96%，去除效率隨著溫度升高而提升，而各操作溫度隨著操作時間從30分鐘增加至60分鐘，去除效率皆未顯著提升；添加5%奈米零價鐵於操作時間60分鐘，250oC、300oC、350oC及400oC之六氯苯去除效率為則為34%、42%、67%及97%，250oC時去除效果優於未添加之情況，然而於350oC去除效率卻較未添加零價鐵為低，顯示加入零價鐵於不同溫度對六氯苯去除效率有不同程度之影響。動態系統未添加零價鐵時，操作時間60分鐘，250oC、300oC、350oC及400oC之六氯苯去除效率為22%、53%、66%及88%，添加5%奈米零價鐵之效率為36%、51%、65%及88%，去除效率隨著溫度升高而提升，和靜態系統之趨勢相同。然而兩系統於添加零價鐵後皆有其他氯數之氯苯生成，其中350oC生成最為顯著。氯苯生成量於400oC大幅降低，顯示此溫度之破壞效率已大於生成效率。零價鐵於熱裂解系統內釋出電子並對六氯苯進行降解，反應後Fe2+及Fe3+可能與土壤中之元素生成金屬催化物，例如FeCl2, FeCl3，催化致使氯苯生成。戴奧辛生成以350oC時最為顯著，以高氯數戴奧辛為主；毒性當量之貢獻以2,3,7,8-TeCDD、1,2,3,7,8-PeCDD及2,3,4,7,8-PeCDF最為顯著，顯示於缺氧情況下，以熱裂解去除土壤中六氯苯之過程仍有戴奧辛生成之潛勢能。然而400oC未見戴奧辛生成，顯示400oC之戴奧辛破壞效率高於生成效率。

摘要(英)

Hexachlorobenzene (HCB) was widely used in agriculture as pesticides. Some of the important characteristics of HCB include low water solubility, bioaccumulation. It is easy to adsorb and difficult to remove from soil. In this study, pyrolysis with static system and dynamic system are applied to treat HCB-contaminated soil, the impact of nanoscale iron on HCB removal will also be evaluated. The results display the HCB removal efficiencies achieved with the static system with temperature varying from 250 to 300, 350oC and 400oC at 60 min without nZVI are 18%, 42%, 74% and 96%, respectively. It displays the benefit of HCB removal at a higher temperature. However, the removal efficiency does not change much as the treatment time is extended from 30 to 60 min. The HCB removal efficiencies achieved with temperature varying from 250 to 300, 350oC and 400oC at 60 min with 5%-nZVI are 34%, 42%, 67% and 97%, respectively. The HCB removal efficiency increases at 250oC if compared with the case without nZVI but decreases at 350oC. It displays that nZVI has different effects on HCB removal at different temperatures. The results obtained with the dynamic system indicate that HCB removal efficiencies achieved with temperature varying from 250 to 300, 350 and 400oC at 60 min without nZVI are 22%, 53%, 66 and 87%, respectively. In the presence of 5%-nZVI, the HCB removal efficiencies achieved are 36%, 51%, 65 and 87%, respectively. These trends are similar to that observed in static system. The results obtained from both static system and dynamic system indicate that CBs are generated when nZVI is added. CBs are generated significantly at 350oC but decreased at 400oC. It indicates that the destruction efficiency is increased significantly at 400oC. Possible reasons of CB generated are that nZVI release electrons and generate other iron-containing compounds, like FeCl2 or FeCl3. Precursors exist in soil may react with chloride to form chlorobenzenes through the catalysis of these iron-containing compounds. PCDD/Fs are generated significantly at 350oC and form higher chlorinated congeners. 2,3,7,8-TeCDD, 1,2,3,7,8-PeCDD and 2,3,4,7,8-PeCDF are the main species contributing to toxicity. On the other hand, formation of PCDD/Fs is not significant for the system operating at 400oC. It indicates that pyrolysis of HCB-contaminated soil also generates PCDD/Fs even oxygen is not provided to the system.

關鍵字(中)

★ 六氯苯
★ 熱裂解
★ 零價鐵
★ 戴奧辛生成

關鍵字(英)

★ Hexachlorobenzene
★ Pyrolysis
★ nZVI
★ PCDD/Fs formation

論文目次

摘要 i
Abstract iii
目錄 v
圖目錄 viii
表目錄 x
第一章前言 1
研究源起及目的 1
第二章文獻回顧 3
2.1 持久性有機污染物 3
2.2 六氯苯 3
2.2.1六氯苯生物毒性 7
2.2.2六氯苯國內外污染案例及法規標準 8
2.3 戴奧辛生成機制 9
2.4 POPS污染土壤整治方法 13
2.5 熱處理技術 15
2.5.1 焚化/燃燒技術 15
2.5.2 熱脫附技術 16
2.5.3 熱裂解技術 18
2.6 各種土壤污染整治技術所需經費之比較 22
2.7 奈米零價鐵特性與發展 23
2.7.1 零價鐵 23
2.7.2 零價鐵還原脫氯機制 24
2.7.3 奈米化零價鐵特性 26
2.7.4 零價鐵合成方式 26
2.8 利用奈米零價鐵去除含氯污染物文獻總述 27
第三章研究方法與設備 31
3.1 污染土壤配置 31
3.2 建立批次熱裂解系統 32
3.3土壤基本特性分析 36
3.3.1元素分析儀 36
3.3.2感應耦合電漿質譜儀法 37
3.4 奈米零價鐵製備及零價鐵分析方法 38
3.4.1 奈米零價鐵合成 38
3.4.2 零價鐵分析方法 39
3.5 土壤中六氯苯及副產物分析 41
3.5.1 索式萃取法 41
3.5.2 淨化程序 42
3.5.3 氯苯分析程序 44
3.6 戴奧辛分析 46
3.6.1 樣品萃取程序 46
3.6.2 淨化程序 46
3.6.3 HRMS分析程序 49
3.7 實驗之藥品、溶劑、材料、設備 55
3.7.1 實驗藥品 55
3.7.2 實驗溶劑 55
3.7.3 實驗材料 55
3.7.4 實驗設備 56
第四章結果與討論 57
4.1 土壤基本特性分析探討 57
4.1.1 土壤中元素分析 57
4.1.2 土壤中氯鹽分析 58
4.2 奈米零價鐵特性分析及其反應性 59
4.2.1 比表面積分析 59
4.2.2 XRD及SEM分析 59
4.3 批次熱裂解探討 61
4.3.1 靜態熱裂解系統對土壤中HCB之去除效率 61
4.3.2 靜態熱裂解後土壤中CBs氣、固相濃度分佈 64
4.3.3 靜態熱裂解後土壤中CBs總濃度分佈 68
4.3.4 動態熱裂解系統對土壤中HCB之去除效率 70
4.3.5 動態熱裂解後土壤中CBs氣、固相濃度分佈 71
4.3.6 靜態及動態熱裂解系統之比較 74
4.3.7 六氯苯降解動力參數 77
4.3.8 氯苯生成機制探討 80
4.3.9 六氯苯污染土壤熱裂解副產物分析 83
4.3.10 熱裂解系統之戴奧辛生成潛能 84
第五章結論與建議 90
5.1 結論 90
5.2 建議 91
參考文獻 92

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指導教授

張木彬(Moo-been Chang)

審核日期

2013-8-23

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