以分層式流體化活性碳床吸附戴奧辛之初步研究

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以分層式流體化活性碳床吸附戴奧辛之初步研究

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摘要(中)

戴奧辛呋喃(PCDD/F)污染在最近年來已成為全世界最重要的環境問題之一，尤其戴奧辛之毒性高且最引人注目，因此世界各國均制定更嚴格之排放標準及最佳控制技術來加以限制戴奧辛的排放及生成。本研究以集塵灰高溫冶煉廠(Waelz process)之萃取液(正壬烷溶液)，作為本研究之進流戴奧辛，以模擬Waelz process戴奧辛之排放特性，選擇以球狀活性碳為實驗之床質吸附劑，並結合分層式流體化床反應器評估在不同氣流流量、操作溫度及水氣含量條件下對戴奧辛吸附效能及戴奧辛前驅物質(氯酚)生成戴奧辛之潛勢及影響。
戴奧辛吸附效率方面，研究結果指出不論在氣流流量、操作溫度及水氣含量條件下，戴奧辛氣流通過第3層時，去除率最高達99.99 %，且毒性當量濃度均已降至0.1 ng-TEQ/Nm3以下，可符合世界最嚴格之法規管制標準。在不同氣流流量條件下，研究結果顯示戴奧辛去除率以7 slpm最高，且戴奧辛去除率均隨氣流流量的提升而呈現下降趨勢。在不同操作溫度條件下，戴奧辛去除率隨著溫度的上升而有下降趨勢。在水氣存在條件下，研究結果顯示水氣存在條件下(0 %、 5 %、10 %及15 %)，通過第一層吸附床之戴奧辛濃度皆超過1 ng-TEQ/Nm3，顯示水氣在活性碳吸附戴奧辛上扮演負面的角色。
本研究亦探討戴奧辛前驅物質(氯酚)在未添加水氣及加入水氣後，通過球狀活性碳吸附床之戴奧辛生成潛勢，研究結果顯示在未添加水氣及加入水氣條件下，戴奧辛總生成量隨著操作溫度的上升而增加，氯酚之轉換率亦隨著操作溫度的升高而增加，呋喃(PCDF)之總生成量比戴奧辛(PCDD)高，此外，操作溫度與戴奧辛生成量成正相關，但不影響戴奧辛生成之物種分佈，水氣條件則使戴奧辛生成物種分佈略有不同，另外，脫附至氣流之戴奧辛濃度(氣相)隨著溫度升高而增加，在200 oC時，戴奧辛濃度(氣相)最高，且戴奧辛物種以低氯數之PCDD及PCDF為主，無水氣條件下，脫附至氣流中之戴奧辛物種以PCDF為主，加入水氣後，脫附至氣流中之戴奧辛除了PCDF之外，亦發現PCDD脫附至氣流中。

摘要(英)

Emission of dioxins has become one of the most important environmental issues in recent years. Due to its high toxicity, the governments worldwide have implemented strict standards to regulate PCDD/F emissions. The objective of this study is to develop a more efficient activated carbon adsorption system. This study employs the bead-shaped activated carbon (BAC) as the adsorbent and combines the laboratory-scale multi-layer fluidized bed reactor to adsorb PCDD/Fs at different operating conditions, including gas flow rates, temperature and water vapor content.
For PCDD/F adsorption experiments, the results indicate the removal efficiency of PCDD/Fs is up to 99.99 % as the PCDD/F-containing gas flow passes through the third layer of the adsorption bed and the outlet PCDD/Fs concentrations would meet the 0.1 ng-TEQ/Nm3 emission standard. The influences of operating conditions on removal efficiency of PCDD/F reveal that the PCDD/F removal efficiency decreases as gas flow rates and operating temperature increase. In addition, the water vapor content plays a negative role in PCDD/F adsorption. In the presence of water vapor, as the PCDD/F-containing gas flow passes through the first layer of the adsorption bed, the outlet PCDD/Fs concentration would exceed 1 ng-TEQ/Nm3 .
Additionally, this study used chlorophenols as precursor to PCDD/F formation. More PCDD/Fs are formed as the operating temperature is increased from 150 oC to 200 oC. In addition, the conversion of chlorophenols increases with increasing operating temperature and the PCDF/PCDD ratio exceeds 1. The operating temperature has positive influence on PCDD/F formation but does not significantly change seventeen 2,3,7,8-substituted PCDD/Fs congeners distribution. The outlet concentration of PCDD/F (gas phase) also increases as operating temperature is increased and the major PCDD/F congeners are lowly chlorinated PCDD/F. In the absence of water vapor, most of the PCDD/Fs in the gas stream are PCDFs (about 98 %). In the presence of water vapor, some PCDDs would desorb to the gas stream.

關鍵字(中)

★ 戴奧辛前驅物質(氯酚)
★ 分層式流體化床反應器
★ 球狀活性碳
★ 戴奧辛

關鍵字(英)

★ PCDD/F
★ multiple layers fluidized bed reactor
★ bead-shaped activated carbon
★ precursor

論文目次

第一章前言 1
1.1 研究緣起 1
1.2 研究目的與範疇 2
第二章文獻回顧 3
2.1 戴奧辛基本特性 3
2.2 戴奧辛來源及生成機制 4
2.2.1 戴奧辛之來源 4
2.2.2 戴奧辛之生成機制 4
2.3 煙道排氣中氣相戴奧辛之控制技術 9
2.3.1 噴入式吸附系統 (Carbon injection) 11
2.3.2 固定床吸附系統 (Fixed-bed) 12
2.3.3 流動床吸附系統 (Moving-bed) 14
2.4 影響活性碳吸附戴奧辛之因素 20
2.4.1 活性碳特性之影響 20
2.4.2 溫度條件之影響 22
2.4.3 水氣條件之影響 24
2.4.4 戴奧辛物種之影響 25
2.5 顆粒體流動性質之量測 25
2.6 流體化床 27
2.6.1 流體化現象 27
2.6.2 實廠化流體化床之相關研究 30
第三章研究方法與步驟 32
3.1 研究流程設計 32
3.2 戴奧辛實驗之藥品、溶劑、材料與設備 35
3.2.1 實驗藥品 35
3.2.2 實驗溶劑 36
3.2.3 實驗材料 36
3.2.4 實驗設備 37
3.3 戴奧辛樣品分析 38
3.3.1 戴奧辛樣品前處理 38
3.3.2 HRMS分析儀器條件設定 43
3.4 實驗設計 46
3.4.1 分層式流體化活性碳吸附床吸附戴奧辛實驗系統之建立 46
3.4.2 反應操作參數 48
3.5 其他儀器原理 49
3.5.1 BET比表面積分析儀 (ASAP2010) 49
3.5.2 掃描式電子顯微鏡分析 (SEM) 49
3.5.3 感應耦合電漿原子發射光譜分析儀 (ICP-AES) 50
3.5.4 流動性質測量 (Jenike剪力測試儀) 51
第四章結果與討論 54
4.1 活性碳基本性質分析 54
4.1.1 比表面積及孔體積 54
4.1.2 掃描式電子顯微鏡 (SEM) 55
4.1.3 感應耦合電漿原子發射光譜分析儀 (ICP-AES) 57
4.1.4 活性碳流動性質量測 (Jenike剪力測試儀) 58
4.1.4.1 壁面摩擦角試驗 58
4.1.4.2 內摩擦角 62
4.2 以經驗式估算最小流體化速度 64
4.3 操作參數之探討 66
4.3.1 進流戴奧辛濃度分析 66
4.3.2 氣流流量對分層式流體化活性碳床去除戴奧辛之影響 68
4.3.3 操作溫度對分層式流體化活性碳床去除戴奧辛之影響 74
4.3.4 水氣含量對分層式流體化活性碳床去除戴奧辛之影響 80
4.3.5 球狀活性碳吸附戴奧辛之質量平衡 84
4.3.5.1 不同氣流流量，球狀活性碳吸附戴奧辛
之質量平衡 84
4.3.5.2 不同操作溫度，球狀活性碳吸附戴奧辛
之質量平衡 89
4.3.5.3 不同水氣含量，球狀活性碳吸附戴奧辛
之質量平衡 93
4.3.6 戴奧辛前驅物質(氯酚)生成戴奧辛之影響 96
第五章結論與建議 104
5.1 結論 104
5.2 建議 106
參考文獻 107

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指導教授

張木彬(Moo-Been Chang)

審核日期

2007-7-24

推文