本研究針對國內兩座燒結廠 (即燒結廠A及B，均配備有靜電集塵器與選擇性觸媒還原)進行煙道氣固相戴奧辛煙道採樣及分析。兩座燒結廠煙道廢氣採樣分析結果，均以靜電集塵器捕集之飛灰戴奧辛濃度作為校正因子以校正之。為了解煙道廢氣中氣固相戴奧辛分布合理性，本研究亦就Chi and Chang (2005)之煙道廢氣中戴奧辛氣固分布推估模式所得結果，與校正前後之煙道廢氣戴奧辛氣相比例進行比對。研究結果發現，校正後之燒結廠A與B之靜電集塵器對戴奧辛去除效率均為固相大於氣相，且去除效率皆為正值 (A：氣相：4.56%；固相：97.8%；B：氣相：63.3%；固相97.3%)，與校正前之去除效率有所差異 (A：氣相：-116%；固相：63.1%； B：氣相：46%；固相：57.5%)。由於燒結廠A與B之煙道廢氣溫度皆低於de novo溫度窗 (<250℃)，其戴奧辛生成機率極低，因此校正後之靜電集塵器去除效率較為合理。本研究亦發現校正後之選擇性觸媒還原對氣相戴奧辛去除效率(A：氣相：62.7%；固相：52.2%； B：氣相：65.5%；固相：-272%)比校正前高 (A：氣相：24.9%；固相：80.7%； B：氣相：-57.1%；固相：95.1%)且均為正值。由於選擇性觸媒還原係藉觸媒表面活性位置與氣相戴奧辛進行氧化反應，進而分解之，因此未校正前B廠之負值並不合理。另由於粒狀物可能吸/脫附出觸媒表面或觸媒老化，造成觸媒剝落，因此可能導致A與B廠之粒狀物去除效率分別為52.2%與-272%，從上述結果可推知，校正後之去除效率應較為合理。校正後排放之煙道廢氣戴奧辛氣固相分布，以氣相戴奧辛為主 (93~99%)，其氣相比例皆比Chi and Chang (2005)之預測模式估算(76~99%)及校正前氣相比例 (71~87%)高，其可能係因煙道廢氣與採樣裝置之溫度差異、粒狀物特徵(濃度與粒徑大小)、及空氣污染防治設備的形式等，導致採樣時氣相戴奧辛吸附於粒狀物表面，進而以固相戴奧辛形式存在。總之，本研究發現以靜電集塵器捕集之飛灰戴奧辛濃度，應足以作為煙道廢氣氣固相戴奧辛分布之校正，亦能有效評估污染防治設備對氣固相戴奧辛之控制效率。

The objective of this study is to establish a new way for correcting gas-particle partitioning of dioxin in flue gas, to discuss its rationality and to know the real dioxin removal efficiency of air pollution control devices (APCDs) in the sinter plant. The two sinter plants investigated are equipped with electrostatic precipitator (EP) and selective catalytic reduction (SCR) system. Partitioning of dioxin between gas and particulate phases in flue gas of the two sinter plants are evaluated via stack sampling and analysis and used the dioxin concentration of EP dust as an adjusted factor. In addition, the prediction model of dioxin partitioning between gas and particulate phases in flue gas published by Chi and Chang (2005) is included in order to discuss further rationality of partitioning of dioxin between gas and particulate phases in flue gas. The results of the removal efficiency of EP show that the adjusted gas-particle partitioning of dioxin are positive (A: gas phase: 4.56%; particulate phase: 97.8%; B: gas phase: 63.3%; particulate phase: 97.3%). The removal efficiency of particulate phase of original (A: gas phase: -116%; particulate phase: 63.1%; B: gas phase: 46.0%; particulate phase: 57.5%) and adjusted gas-particle partitioning of dioxin are higher than gas phase. Because the temperatures of flue gas are out of de novo synthesis, dioxin wouldn’t be formatted in the flue gas. Therefore, the removal efficiency of EP of adjusted gas-particle partitioning of dioxin should be more rationality. In addition, the results of removal efficiency of SCR show that the dioxin removal efficiency of particulate phase of original gas-particle partitioning are higher than gas phase (A: gas phase: 39.9%; particulate phase: 85.5%; B: gas phase: 95.1%; particulate phase: -57.1%), but the results of removal efficiency of adjusted gas-particle partitioning are contrary (A: gas phase: 62.7%; particulate phase: 52.2%; B: gas phase: 65.5%; particulate phase: -272%). In the SCR, dioxins of gas phase are reacted on the catalyst with oxygen and are converted into harmless carbon dioxide and water. Therefore, the negative removal efficiency of gas phase of the original gas-particle partitioning of dioxin is not rational. The particle would be adsorbed/desorbed from catalytic surface in the SCR, and caused the removal efficiency of particle are 52.2% and -272% in the sinter plant A and B, respectively. Based on those results, the removal efficiency of adjusting gas-particle partitioning of dioxin should be more rational. After adjusting gas-particle partitioning of dioxin, the dioxin of flue gas are mostly distributed in gas phase (93~99%) in the two sinter plants investigated. The gaseous ratios of adjusted gas-particle partitioning of dioxin are higher than the predicted (76~99%) and the original gas-particle partitioning of dioxin (71~87%). Those differences may cased by the difference of temperature between flue gas and sampling device, the characteristics of particle (concentration and size distribution), and the type of applied APCDs. Therefore, it caused severe adsorption of gaseous onto particles while sampling and caused the mis-estimation of the predicted gaseous ratios. Overall, this study provides important references for the correcting method of gas-particle partitioning of dioxin in the sinter flue gas and effective evaluating the removal efficiency of APCDs.

摘要 i
Abstract ii
致謝 iii
目 錄 iv
表目錄 vi
第一章 緒論 1
1-1 研究緣起 1
第二章 文獻回顧 2
2-1 戴奧辛物理化學特性 2
2-2 戴奧辛造成的健康不良效應 2
2-3 戴奧辛生成機制 4
2-4 環境中戴奧辛之來源 5
2-5 戴奧辛控制技術 6
2-6 戴奧辛濃度氣固相分布 8
2-6-1 戴奧辛濃度氣固相分布重要性 8
2-6-2 煙道廢氣戴奧辛氣固相採樣方法發展 8
2-6-3 氣固相戴奧辛分布預估模式 9
2-6-4 煙道採樣存在之問題 9
第三章 實驗材料與方法 19
3-1-0 研究架構 19
3-1-1 研究假設與研究對象選取條件 19
3-1-2 研究對象 20
3-2 採樣位置 20
3-3 煙道採樣 20
3-3-1採樣設備 20
3-3-2煙道PCDD/Fs採樣器抽氣體積計算 21
3-4 PCDD/Fs煙道廢氣採樣方法 24
3-5 PCDD/Fs樣品之前處理 29
3-6 儀器分析 32
3-7 品質保證及品質控制 33
3-7-1 實驗藥品與試劑 33
3-7-2 採樣品質保證與品質控制之執行 35
3-7-3 PCDD/Fs樣品分析前處理品質保證與品質控制之執行 36
3-8 PCDD/Fs於不同溫度下蒸氣壓計算方法 37
3-9 煙道廢氣中PCDD/Fs濃度之校正方式 37
第四章 結果與討論 52
4-1 煙道廢氣基本組成特徵 52
4-2 校正前之燒結廠煙道廢氣PCDD/Fs濃度、特徵剖面及APCDs對其之去除效率 53
4-2-1 校正前之煙道廢氣PCDD/Fs濃度 53
4-2-2 校正前之煙道廢氣PCDD/Fs之特徵剖面 54
4-2-3 校正前燒結廠APCDs對PCDD/Fs去除效率 56
4-3 Chi與Chang (2005)模式推估之燒結廠煙道廢氣PCDD/Fs濃度及APCDs對其之去除效率 57
4-3-1 PCDD/Fs蒸氣壓與戴奧辛氣固相關係 57
4-3-2 Chi與Chang (2005)模式推估之燒結廠煙道廢氣PCDD/Fs濃度 58
4-3-3 經Chi與Chang (2005)模式推估煙道廢氣氣固相PCDD/Fs濃度分布後之APCDs去除效率 58
4-4 經EP飛灰校正燒結廠煙道廢氣氣固相PCDD/Fs濃度後之煙道廢氣PCDD/Fs濃度與APCDs去除效率 59
4-4-1 EP飛灰中PCDD/Fs濃度與特徵剖面 59
4-4-2 校正前之燒結廠煙道廢氣固相PCDD/Fs與EP飛灰固相PCDD/Fs濃度比較 60
4-4-3 經校正後燒結爐煙道廢氣PCDD/Fs之濃度 61
4-4-4 經校正燒結廠煙道廢氣氣固相PCDD/Fs濃度分布後之APCDs去除效率 62
4-5 APCDs去除效率與PCDD/Fs氣相分布比例比較與合理性探討 62
4-5-1 APCDs去除效率比較與合理性探討 63
4-5-2 煙道PCDD/Fs氣相分布比例比較與合理性探討 65
第五章 結論與建議 97
5-1 結論 97
5-2 建議 97
第六章 參考文獻 98

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