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系統識別號 U0026-1307201222550900
論文名稱(中文) 農廢露天燃燒及固定污染源排放半揮發性有機污染物之特徵
論文名稱(英文) Characteristics of Semi-Volatile Organic Compounds in the Biomass Open Burning and from the Stationary Sources
校院名稱 成功大學
系所名稱(中) 資源工程學系碩博士班
系所名稱(英) Department of Resources Engineering
學年度 100
學期 2
出版年 101
研究生(中文) 邱瑞基
研究生(英文) Jui-Chi Chiu
學號 n48931108
學位類別 博士
語文別 英文
論文頁數 75頁
口試委員 指導教授-申永輝
召集委員-李文智
口試委員-陳瑞仁
口試委員-楊錫賢
口試委員-蔡政賢
口試委員-王琳麒
中文關鍵字 戴奧辛  呋喃  多環芳香烴化合物  乾沉降  煙道氣  排放係數  指紋鑑別物種 
英文關鍵字 Dioxins  Furans  PAHs  BaPeq  Dry deposition  Flue gas  Emission factor  Indicatory congeners 
學科別分類
中文摘要 本研究係針對不同污染源排放多環芳香烴化合物及戴奧辛/呋喃特徵進行研究,內容分為二大部份:第一部分藉由代表性稻田在農業廢棄物露天燃燒及非露天燃燒期間之採樣分析,求得大氣中懸浮微粒與多環芳香烴化合物之濃度與特徵剖面。本研究區域為臺灣農廢露天燃燒盛行地區之嘉南平原,進行多環芳香烴化合物在露天燃燒前期、高峰期與後期周界大氣中之濃度建立,解析農廢露天燃燒排放多環芳香烴化合物特徵,對周界大氣中多環芳香烴化合物之影響程度。分析數據顯示,稻田非露天燃燒期間,大氣中總多環芳香烴化合物和BaPeq的平均濃度分別為376和 1.50 ng/m3、平均乾沉降通量分別為1222和 4.80 µg/m2-day;而稻田農廢露天燃燒高峰期間,周界大氣中總多環芳香烴化合物和BaPeq的平均濃度分別增加19倍(7206 ng/m3)及6.8倍( 10.3 ng/m3),平均乾沉降通量增加了60倍及3倍,可見農廢露天燃燒對周界大氣多環芳香烴化合物濃度造成顯著增加,以毒性觀點論之,總BaPeq的增加也提高了致癌的風險度。在稻田非露天燃燒期間,總多環芳香烴化合物的乾沉降通量貢獻中,粒狀多環芳香烴化合物佔了79.2~ 84.2%;然而稻田農廢露天燃燒高峰期間,乾沉降通量中粒狀多環芳香烴化合物提升至85.9~ 95.5%。這結果顯示稻田農廢露天燃燒使大氣中懸浮微粒的含量增加,也同時讓總多環芳香烴化合物的乾沉降通量明顯增加。
第二部分針對南臺灣操作運轉中之金屬冶煉業、火葬場及廟宇金爐等可能排放戴奧辛/呋喃之特定固定污染源,進行煙道廢氣排放戴奧辛/呋喃採樣分析研究,包括一座電弧爐、一座鋁二級冶煉廠、一座火葬場及二座廟宇金爐;除火葬場外,每座固定空氣污染源採集爐室底渣及空氣污染防制設備飛灰樣品,進行戴奧辛/呋喃之分析。電弧爐、鋁二級冶煉廠、火葬場與廟宇金爐煙道廢氣中總PCDD/Fs I-TEQ濃度介於0.00681及0.703 ng I-TEQ/Nm3之間,排放係數介於0.00827及3.50 μg I-TEQ/ton。電弧爐、鋁二級冶煉廠底渣中總PCDD/Fs I-TEQ含量分別為21.3及0.494 ng I-TEQ/kg,而飛灰中總PCDD/Fs I-TEQ含量分別為74.0及49.9 ng I-TEQ/kg。同時因為記憶效應(memory effect),電弧爐袋式集塵器的PCDD/Fs去除效率為 -44.4%。電弧爐、鋁二級冶煉廠煙道中PCDD/Fs之特徵剖面相似(1,2,3,7,8,9-HxCDF、2,3,7,8-TeCDF及1,2,3,7,8-PeCDF)。此外,火葬場與廟宇金爐煙道廢氣中PCDD/Fs之特徵剖面相似(2,3,4,6,7,8-HxCDF、OCDF、1,2,3,4,6,7,8- HpCDD及OCDD)。金屬工業(電弧爐、鋁二級冶煉廠)的PCDD/Fs排放源貢獻量主要來自於飛灰(佔61.1~95.3%) ,而廟宇金爐則以煙道排氣的PCDD/Fs排放貢獻最大(99.9%)。綜上,為掌握並了解PCDD/Fs的排放現況,必須持續監控不同排放源(煙道/飛灰/底渣)與既有空氣污染防制設備,並建立PCDD/Fs的排放源資料及主要指紋鑑別物種,有助於後續針對不同特性排放源提供有效管制策略。
英文摘要 The objectives of the research were to investigate polycyclic aromatic hydrocarbons (PAHs) and polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) characteristics from the emission sources. It contains two parts: the first part of this study includes the particulate matter (PM) and PAHs concentrations during rice straw open burning and non-open burning periods. In the ambient air of a rice field, the mean total PAH and total toxic equivalence (BaPeq) concentrations were 7206 ng/m3 and 10.3 ng/m3, respectively, whereas after the open burning event, they were 376 ng/m3 and 1.50 ng/m3, respectively. Open burning thus increases total PAH and total BaPeq concentrations by 19-fold and 6.8-fold, respectively. During a rice straw open burning event, in the ambient air of a rice field, the mean dry deposition fluxes of total PAHs and total BaPeq were 1222 µg/m2-day and 4.80 µg/m2-day, respectively, which are approximately 60- and 3-fold higher than those during the non-open burning period, respectively. During the non-open burning period, particle-bound PAHs contributed 79.2-84.2% of total dry deposition fluxes (gas + particle) of total PAHs. However, an open burning event increases the contribution to total PAH dry deposition by particle-bound PAHs up to 85.9-95.5%. The results show that due to the increased amount of PM in the ambient air resulting from rice straw open burning, particle-bound PAHs contributed more to dry deposition fluxes of total PAHs than they do during non-open burning periods. The results show that biomass (rice straw) open burning is an important PAH emission source that significantly increases both PM and PAH concentration levels and PAH dry deposition in ambient air.
The second part is set out to clarify the emissions and distribution of PCDD/Fs from the stack flue gases, fly ashes and bottom ashes of various stationary sources. The mean total PCDD/F I-TEQ concentration of flue gas ranged from 0.00681 to 0.703 ng I-TEQ/Nm3. However, the emission factor of PCDD/F from various incinerators was 0.00827 to 3.50 µg I-TEQ/ton, whereas it was 5.36 µg I-TEQ/body for a crematory (CM). In addition, the mean total PCDD/F I-TEQ content in fly ash from an electric arc furnace (EAF) and a secondary aluminum smelter (secondary ALS) were 74.0 and 49.9 ng I-TEQ/kg, respectively, whereas they are 21.3 and 0.494 ng I-TEQ/kg for bottom ash. Meanwhile, the removal efficiency of PCDD/F by bag filters from EAF was -44.4% which is attributed to the “memory effect”. The indicatory PCDD/Fs of EAF, and secondary ALS have the same congeners (1,2,3,7,8,9-HxCDF, 2,3,7,8-TeCDF, and 1,2,3,7,8-PeCDF). In addition, CM, joss paper-A (JP-A) and joss paper-B (JP-B) incinerators have similar indicatory PCDD/F (2,3,4,6,7,8-HxCDF, OCDF, 1,2,3,4,6,7,8-HpCDD, and OCDD). The high contribution of total PCDD/F is from fly ash (61.1-95.3%) for metallurgical facilities (EAF, secondary ALS), whereas 99.9% contribution of stack flue gas is from JP-A and JP-B. In conclusion, continually monitoring various PCDD/F emission sources is necessary to understand current PCDD/F emission (flue gas, fly/bottom ash) and the related removal efficiency of existing air pollution control devices. Information about both emission factors of PCDD/Fs and indicatory PCDD/F congeners are useful for the establishment of control strategies and for use as fingerprints with regard to the dominant congeners from different emission sources.
論文目次 Contents/ 總目錄
Abstract..........................................I
摘要..............................................IV
Acknowledgements/ 誌謝...........................VII
Contents/ 總目錄................................VIII
List of tables/ 表目錄............................XI
List of figures/ 圖目錄.........................XIII
Chapter 1 Introduction...........................1
Chapter 2 Literature Review......................5
2.1 PCDD/Fs......................................5
2.1.1 Physical and chemical properties...........5
2.1.2 Health and environmental effects...........6
2.1.3 Formation mechanisms.......................8
2.1.4 Control technologies of PCDD/Fs emission...9
2.1.5 Emission inventory........................10
2.2 PAHs........................................13
2.2.1 Physical and chemical properties..........13
2.2.2 Health and environmental effects..........14
2.2.3 Transportation and contribution...........15
2.2.4 Biomass burning...........................17
Chapter 3 Research Methodology..................19
3.1 The Procedure of the experiments............19
3.2 Sampling....................................23
3.2.1 Sampling of PAHs..........................23
3.2.2 Sampling of PCDD/Fs.......................23
3.3 Analysis....................................24
3.3.1 Analysis of PAHs..........................24
3.3.2 Analysis of PCDD/Fs.......................25
3.4 Gas/particle partitioning...................26
3.5 Dry deposition of PAHs......................27
3.6 Indicatory PCDD/Fs..........................28
Chapter 4 Results and Discussion................30
4.1 Properties of rice straw....................30
4.2 PM and PAH concentrations in ambient air before, during,and after open burning period.............31
4.3 PM and PAH concentration in ambient air during and after open burning event at a rice field and air quality monitoring station...............................33
4.4 Gas/particle partitioning of PAHs...........37
4.5 Dry deposition of PAHs......................38
4.6 PCDD/F concentrations in the stack flue gas.42
4.7 Emission factors of various PCDD/F sources..46
4.8 PCDD/F contents in fly ash and bottom ash...48
4.9 PCDD/F removal efficiency by bag filter.....51
4.10 Indicatory PCDD/Fs.........................51
4.11 The fate of PCDD/Fs........................53
Chapter 5 Conclusions and Recommendations.......54
5.1 Conclusions.................................54
5.2 Recommendations.............................56
REFERENCES.......................................58
Résumé(自述)......................................71
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