銅污泥處理程序之戴奧辛類化合物與多環芳香烴排放特性探討

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方子翌(Tzu-Yi Fang) 查詢紙本館藏

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論文名稱

銅污泥處理程序之戴奧辛類化合物與多環芳香烴排放特性探討
(Characteristics of Dioxin-like Compounds and Polycyclic Aromatic Hydrocarbons Emitted from Copper-containing Sludge Treatment Process)

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摘要(中)

本研究調查銅污泥處理廠之多氯聯苯戴奧辛及呋喃(Polychlorinated dibenzo-p-dioxins/furans, PCDD/Fs)、戴奧辛類多氯聯苯(dioxin-like Polychlorinated biphenyls, dl-PCBs)及多環芳香烴(Polycyclic Aromatic Hydrocarbons, PAHs)之排放濃度與物種分佈特性，藉由調整空氣污染防制設備(Air Pollution Control Devices, APCDs)操作參數，探討各物種間之去除效率。結果顯示煙囪排氣之PCDD/Fs毒性當量濃度為4.45 - 8.10 ng I-TEQ/Nm3，超過固定污染源之法規管制標準(0.5 ng I-TEQ/Nm3)，dl-PCBs及PAHs量測結果分別為0.617 - 1.60 ng WHO2005-TEQ/Nm3及89.7 - 695 ng BaPeq/Nm3；飛灰及底渣之PCDD/Fs毒性當量濃度亦超過台灣有害事業廢棄物認定標準(1.0 ng-TEQ g-1)，需妥善處理。排氣及灰份之PCDD/Fs物種毒性當量均以2,3,4,7,8PeDF及1,2,3,7,8,9HxDF為主要貢獻物種；而dl-PCBs物種毒性當量則以PeCB-126佔比最高；排氣之PAHs物種毒性當量分佈以BcFE及DBalP佔比最高，灰份之PAHs物種毒性當量分佈則以BcFE、5-MC、BaP及DBalP為主。此外，二燃室＋驟冷塔對PCDD/Fs、dl-PCBs及PAHs之去除效率分別達97%、90%及70%；相對而言，熱交換器+袋式集塵器及洗滌塔對於PCDD/Fs及dl-PCBs有不減反增之趨勢，研究結果發現吸附於熱交換器沉積物之PCDD/Fs及dl-PCBs脫附至氣相導致袋式集塵器出口濃度升高，而洗滌塔因記憶效應導致煙囪排氣之PCDD/Fs及dl-PCBs濃度升高，應審慎考量其存在之必要性。

摘要(英)

The characteristics of PCDD/Fs, dl-PCBs and PAHs emitted from a copper-containing sludge treatment plant are investigated in this study. The removal efficiencies of PCDD/Fs, dl-PCBs and PAHs achieved with APCDs are evaluated via simultaneous sampling at inlet and outlet of APCDs. The results indicate that the TEQ concentration of PCDD/Fs at stack is 4.45 - 8.10 ng I-TEQ/Nm3, which exceeds the Dioxin Emission Standards for Stationary Pollution Sources (0.5 ng I-TEQ/Nm3). The TEQ concentration of dl-PCBs and PAHs at stack are 0.617 - 1.60 ng WHO2005-TEQ/Nm3 and 89.7 - 695 ng BaPeq/Nm3, respectively. In addition, the PCDD/Fs TEQ concentrations of fly ash and bottom ash also exceed the Standards for Defining Hazardous Industrial Waste (1.0 ng-TEQ g-1), which should be properly treated. Moreover, in both stack and ash, 2,3,4,7,8PeDF and 1,2,3,7,8,9HxDF are the main TEQ contrubution, while PeCB-126 is the donminant congener of dl-PCBs. As for PAHs, BcFE and DBalP are the highest TEQ distribution in exhaust gas, while BcFE, 5-MC, BaP and DBalP are dominant in ash. In addition, the removal efficiencies of PCDD/Fs, dl-PCBs and PAHs achieved with SCC + QT reach 97%, 90% and 70%, respectively. However, the concentration of PCDD/Fs and dl-PCBs after heat exchanger+BH and WS increase. PCDD/Fs and dl-PCBs are desorbed to the gas phase in the heat exchanger, causing the increase of concentration after heat exchanger+BH. Besides, the concentration of PCDD/Fs and dl-PCBs increase across the WS is due to the memory effect. The necessity of its existence should be carefully considered.

關鍵字(中)

★ 戴奧辛及呋喃
★ 多氯聯苯
★ 多環芳香烴
★ 銅污泥處理廠
★ 毒性當量濃度

關鍵字(英)

★ Polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs)
★ dioxin-like Polychlorinated biphenyls (dl-PCBs)
★ Polycyclic Aromatic Hydrocarbons (PAHs)
★ copper-containing sludge treatment plant
★ toxicity equivalent concentration (TEQ

論文目次

摘要 I
ABSTRACT II
目錄 III
圖目錄 VI
表目錄 X
第一章前言 1
1-1 研究緣起 1
1-2 研究目的 1
第二章文獻回顧 3
2-1 戴奧辛類化合物與多環芳香烴之特性 3
2-1-1 戴奧辛類化合物之特性 3
2-1-2 多環芳香烴之特性 4
2-2 熱處理過程中PCDD/FS及DL-PCBS的生成機制 6
2-2-1 均相(氣相)反應 6
2-2-2 異相(固相)反應 7
2-2-3 由前驅物形成之PCDD/Fs 7
2-2-4 由De Novo合成反應形成之PCDD/Fs 8
2-2-5 記憶效應 10
2-3 熱處理程序之戴奧辛類化合物排放 12
2-3-1 二次銅冶煉廠之PCDD/Fs及dl-PCBs排放 14
2-3-2 二次銅、鉛及鋅冶煉廠之PCDD/Fs排放 17
2-3-3 二次鋁冶煉廠之PCDD/Fs排放 18
2-3-4 二次鋁冶煉廠之PAHs排放 20
2-3-5 鎂冶煉廠之PCDD/Fs與dl-PCBs排放 22
2-3-6 鎂冶煉廠之PAHs排放 24
2-4 空氣污染防制設備(APCDS)之操作參數對污染物之影響 26
2-4-1 鍋爐燃燒區溫度對PCDD/Fs生成潛勢之影響 26
2-4-2 驟冷塔對PCDD/Fs生成之影響 27
2-4-3 二次燃燒室操作溫度對PCDD/Fs生成之影響 28
2-4-4 洗滌塔對PCDD/Fs生成之影響 29
2-4-5 活性碳噴注量對PCDD/Fs生成之影響 30
第三章研究方法 32
3-1 研究流程及架構 32
3-2 採樣對象 33
3-3 樣品採樣程序 35
3-3-1 煙道氣中戴奧辛類化合物、多環芳香烴及氯化氫採樣程序 35
3-3-2 灰份樣品採樣程序 36
3-4 實驗材料、設備及試劑 37
3-4-1 實驗材料 37
3-4-2 實驗設備 38
3-4-3 實驗試劑 38
3-5 樣品前處理與分析方法 40
3-5-1 煙道氣戴奧辛類化合物樣品萃取程序 40
3-5-2 煙道氣多環芳香烴樣品萃取程序 42
3-5-3 底渣及飛灰樣品萃取程序 44
3-5-4 戴奧辛類化合物樣品淨化程序 44
3-5-5 多環芳香烴樣品淨化程序 45
3-5-6 高解析氣相層析/高解析質譜儀(HRGC/HRMS)分析 46
3-5-7 高解析氣相層析/低解析質譜儀(HRGC/LRMS)分析 48
3-6 其他檢測方法 51
3-6-1 煙道排氣之氣體組成分析 51
3-6-2 氯化氫 52
3-6-3 粒狀物 53
第四章結果與討論 54
4-1 煙道氣採樣基本參數 54
4-2 戴奧辛(PCDD/FS)濃度 56
4-2-1 煙道排氣中戴奧辛濃度 56
4-2-2 煙道排氣中戴奧辛質量濃度之氣固比與PCDD/PCDF分佈 58
4-2-3 煙道排氣中戴奧辛物種質量濃度與毒性當量濃度分佈 60
4-2-4 灰份中戴奧辛濃度 69
4-2-5 灰份中戴奧辛質量濃度之PCDD/PCDF分佈 71
4-2-6 灰份中戴奧辛物種分佈 72
4-2-7 戴奧辛排放係數 82
4-3 多氯聯苯(DL-PCBS)濃度 83
4-3-1 煙道排氣之多氯聯苯濃度 83
4-3-2 煙道排氣中多氯聯苯質量濃度之氣固相分佈 85
4-3-3 煙道排氣中多氯聯苯物種質量與毒性當量濃度分佈 87
4-3-4 灰份中多氯聯苯濃度 95
4-3-5 灰份中多氯聯苯物種質量濃度與毒性當量濃度分佈 97
4-3-6 多氯聯苯排放係數 107
4-4 多環芳香烴(PAHS)濃度 109
4-4-1 煙道排氣中多環芳香烴濃度 109
4-4-2 煙道排氣中多環芳香烴質量濃度之氣固分佈及環數分佈比率 111
4-4-3 煙道排氣中多環芳香烴物種質量濃度與毒性當量濃度分佈 114
4-4-4 灰份中多環芳香烴濃度 122
4-4-5 灰份中多環芳香烴質量濃度之環數分佈比率 124
4-4-6 灰份中多環芳香烴物種質量濃度與毒性當量濃度分佈 124
4-4-7 多環芳香烴排放係數 135
4-5 戴奧辛類化合物與多環芳香烴之質量流佈 136
4-6 多環芳香烴與戴奧辛類化合物質量濃度之相關係數 138
4-7 金屬冶煉業之戴奧辛類化合物之毒性當量比較 139
第五章結論與建議 142
5-1 結論 142
5-2 建議 143
參考文獻 144
附錄一煙道氣樣品之戴奧辛類化合物及多環芳香烴質量濃度 154
附錄二煙道氣樣品之戴奧辛類化合物及多環芳香烴毒性當量濃度 160
附錄三灰份樣品之戴奧辛類化合物及多環芳香烴質量濃度 167
附錄四灰份樣品之戴奧辛類化合物及多環芳香烴毒性當量濃度 173
附錄五煙道氣樣品之戴奧辛類化合物及多環芳香烴回收率 179
附錄六灰份樣品之戴奧辛類化合物及多環芳香烴回收率 183

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張書豪、洪保鎮、張木彬，“含銅污泥資源化過程中戴奧辛物種分布特性檢測研究期末報告”，中央大學環境工程研究所，2008。
行政院環保署，公私場所固定污染源申報空氣污染防制費之粒狀污染物、鉛、鎘、汞、砷、六價鉻、戴奧辛排放係數、控制效率及其他計量規定，2018。

指導教授

張木彬(Moo-Been Chang)

審核日期

2020-8-24

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