臺灣博碩士論文加值系統

本研究為探討台中科技走廊戴奧辛濃度與污染來源長期趨勢，以及釐清該地區之氣團傳輸現象情況。本研究於2009~2014年間進行環境中戴奧辛採樣，並應用化學質量平衡空氣品質模式(CMB-8.2)深入探討戴奧辛之污染來源及其貢獻量，其中本研究建立中部地區11個戴奧辛污染源指紋庫，做為受體模式模擬所需。另外，亦運用軌跡模式(HYSPLIT Model)來探討區域內與鄰近地區大氣中戴奧辛傳輸與影響。
戴奧辛檢測結果與CMB-8.2模擬污染來源之長期趨勢變化，將研究分為三個期程，早期(2009~2010年度)、中期(2011~2012年度)與近期(2013~2014年度)。早期、中期及近期檢測結果分別為0.024~0.123、0.025~0.225與0.012~0.101 pg I-TEQ/m3，其戴奧辛檢測結果有逐年降低的趨勢，在2014年第四次採樣，三個採樣點濃度值都是歷年來最低。模擬貢獻污染源結果在早期主要為垃圾焚化爐與二次煉銅業、中期為垃圾焚化爐與燃煤火力發電廠，以及近期主要為垃圾焚化爐與火葬場。火葬場貢獻比例逐年增加的趨勢，貢獻量較低的來源為醫療焚化爐與廢灰渣處理業，而DC電弧爐業、二次煉鋁業與廢水處理廠幾乎沒有貢獻量。軌跡模擬結果顯示，在逆軌跡氣團大多為東北往西南方傳輸，且逆軌跡缐大多通過垃圾焚化廠之後到達採樣點。推估戴奧辛可能受到位於研究區域的東北方兩座垃圾焚化廠所排放之污染物影響，這明確運用CMB與軌跡模式模擬結果有相關性。

In this study, the chemical mass balance model (CMB8.2) of field measurements of 11 kinds of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) emission sources and ambient air at three sites during 2009-2014 was used to identify the source and relative contribution of ambient PCDD/Fs for a long-term in the Dadu Tableland Technology Corridor. The analysis data of flue gas of 11 kinds of emission sources by four environmental protection bureaus in centre Taiwan were used to establish the exhaust fingerprints of PCDD/Fs from those sources. Additionally, HYSPLIT Trajectory Model was also used to investigate the transport of ambient PCDD/Fs in study area.
The period (2009-2014) was delimited three stages, namely early (2009~2010), middle (2011-2012), and recently (2013-2014) stages, for investigation the variations of temporal and spatial PCDD/Fs distributions in study area. The results of field measurements show that the ranges of ambient PCDD/Fs concentration during early, middle, and recently stages were 0.024-0.123, 0.025-0.225, and 0.012-0.101 pg I-TEQ/m3, respectively. It shows that ambient PCDD/Fs concentration decreases year by year in the Dadu Tableland Technology Corridor. The major contribution sources of PCDD/Fs during early, middle, and recently stages were municipal waste incinerators (MUWI) and secondary copper smelting plants (SCS), MUWI and coal-fired power plants (CFP), and MUWI and crematoria, respectively. Remarkable, the contribution of PCDD/Fs from crematoria increases year by year obviously. Medical waste incinerators (MEWI) and ash treatment plants (AT) were minor contribution sources of PCDD/Fs during each stage. The contributions of PCDD/Fs from DC electric arc furnaces (DEAF), secondary aluminum smelting plants (SAS), and wastewater treatment plants (WT) were very low, with the contribution amounts close to zero. The results of backward trajectory modeling at three sampling sets point out that the main transport path of air mass were from northeast to southwest. Therefore, the major PCDD/Fs emission sources are located on the northeastern of study area, which are the two MUWIs. It shows that the modeling results of chemical mass balance and trajectory models are corresponding. Keywords: PCDD/Fs, CMB8.2, Trajectory model, Temporal and spatial PCDD/Fs distributions.

摘要 .................................................................................................................... i
Abstract ............................................................................................................. ii
目錄 .................................................................................................................. iv
圖目錄 .............................................................................................................. vi
表目錄 .............................................................................................................. ix
第一章 前言 ..................................................................................................... 1
1.1 研究緣起與目的 ................................................................................ 1
1.2 研究架構與內容 ................................................................................ 3
第二章 文獻回顧 ............................................................................................. 5
2.1 地理環境 ............................................................................................ 5
2.2 戴奧辛 ................................................................................................ 7
2.2.1 戴奧辛來源 ................................................................................. 10
2.2.2 環境中戴奧辛現況 ..................................................................... 14
2.3 受體模式之應用 ............................................................................... 19
2.4 軌跡模式之應用 ............................................................................... 22
第三章 研究方法 ........................................................................................... 25
3.1 研究範圍 ........................................................................................... 25
3.2 戴奧辛採樣 ....................................................................................... 28
3.2.1 PS-1 高流量採樣器 .................................................................... 28
3.2.2 戴奧辛分析 ................................................................................. 30
3.2.3 品保品管 ..................................................................................... 37
3.3 受體模式之模擬 ............................................................................... 40
3.3.1 受體模式之基本原理 ................................................................. 40
3.3.2 受體模式之驗證 ......................................................................... 43
台中科技走廊戴奧辛長期濃度與來源趨勢變化探討
逢甲大學 e-Thesys v & Dissertations(103 學年度)
3.3.3 受體模式之操作 ......................................................................... 44
3.4 軌跡模式之模擬 ............................................................................... 45
3.4.1 軌跡模式之基本原理 ................................................................. 45
3.4.2 軌跡模式之操作 ......................................................................... 48
第四章 結果與討論 ....................................................................................... 51
4.1 戴奧辛之採樣分析結果 ................................................................... 51
4.1.1 採樣時段之風向風速與溫度濕度............................................. 52
4.1.2 環境中戴奧辛之歷年濃度趨勢變化探討 ................................ 69
4.2 受體模式探討 ................................................................................... 84
4.2.1 中部地區戴奧辛排放源指紋庫................................................. 84
4.2.2 戴奧辛CMB-8.2模擬歷年結果 ............................................... 88
4.3 軌跡模擬結果 ................................................................................... 98
4.4 探討台中科技走廊戴奧辛長期濃度與來源趨勢變化 ................. 214
第五章 結論與建議 ..................................................................................... 216
5.1 結論 ................................................................................................. 216
5.2 建議 ................................................................................................. 217
參考文獻 ....................................................................................................... 216
附錄1 PCDD/Fs濃度
附錄2 CMB-8.2驗證值

1. 內政部統計處，。http://www.moi.gov.tw/stat/index.aspx
2. 劉璧甄，『大肚山科技走廊大氣微粒之成分解析與來源探討』，碩士論文，逢甲大學環境工程研究所，2009。
3. 黃肇凱，『運用受體模式探討地形與季風條件在揮發性有機物與戴奧辛之大氣濃度及傳輸上的影響』，博士論文，逢甲大學環境工程研究所，2010。
4. T. Chen, X.D. Li, J.H. Yan, S.Y. Lu, K. Cen, Distribution of polychlorinated dibenzo-p-dioxins and dibenzofurans in ambient air of different regions in China. Atmospheric Environment, 45 (2011) 6567-6575
5. 王琳麒、李文智，『污染源及大氣中戴奧辛/呋喃之特徵』，博士論文，國立成功大學環境工程研究所，2003。
6. M.R. Chao, C.W. Hu, Y.L. Chen, G.P. Chang-Chien, W.J. Lee, L.W. Chang, W.S. Lee, K.Y. Wu, Approaching gas-particle partitioning equilibrium of atmospheric PCDD/Fs with increasing distance from an incinerator: measurements and observations on modeling. Atmospheric Environment, 38 (2004) 1501-1510.
7. K.M. Yu, W.J. Lee, P.J. Tsai, K. Fang, M. Lin, Emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) from both of point and area sources of an electric-arc furnace-dust treatment plant and their impacts to the vicinity environments. Chemosphere, 80 (2010) 1131-1136.
8. 行政院環境保護署環境檢驗所，戴奧辛的生物毒性簡介。
9. 日本環境省，関係省庁共通パンフレット『ダイオキシン類』http://www.env.go.jp/chemi/dioxin/pamph/2012.pdf.
10. H. Vogg, H. Hunsinger, A. Merz, L. Stieglitz, Influencing the Production of Dioxin/Furan in Solid Waste Incineration Plants by Measures Affecting the Combustion as well as the Flue Gas Cleaning Systems. Chemosphere, 25 (1992) 149-152.
11. G. Zhang, J. Hai, J. Cheng, Characterization and mass balance of dioxin from a large-scale municipal solid wast incinetator in China. Waste Management, 32 (2012) 1156-1162.
12. J.Y. Ryu, K.C. Choi, J.A. Mullholland, Polychlorinated dibenzo-p-dioxin (PCDD) and dibenzofuran (PCDF) isomer patterns from municipal waste combustion: Formation mechanism fingerprints. Chemosphere, 65 (2006) 1526-1536.
13. J.Y. Ryu, J.A. Mullholland, M. Takeuchi, D.H. Kim, T. Hatanaka, CuCl2-catalyzed PCDD/F formation and congener patterns from phenols. Chemosphere 61(2005) 1312-1326.
14. 日本厚生労働省，生活衛生対策『火葬場から排出されるダイオキシン類削減対策指針』http://www.mhlw.go.jp/bunya/kenkou/seikatsu-eisei19/pdf/01.pdf.
15. N. Takeda, M. Takaoka, T. Fujiwara, H. Takeyama, S. Eguchi, PCDDs/DFs emissions from crematories in Japan. Chemosphere, 40 (2000) 575-586.
16. A. Hoyos, M. Cobo, B. Aristizabal, F. Cordoba, C. M. Correa, Total suspended particulate (TSP), polychlorinated dibenzodioxin (PCDD) and polychlorinated dibenzofuran (PCDF) emissions from medical waste incinerators in Antioquia, Colombia. Chemosphere, 73 (2008) 137-142.
17. 台灣行政院環保署戴奧辛環境毒理簡介
18. J. Ferrario, C. Byrne, D. Cleverly, Summary of Evidence for the Possible Natural Formation of Dixoins in Mined Clay Products. International Symposium on Halogenated Environmental Organic Pollutants and POPs (2000).
19. P. Piccinini, P. Pichat, C. Guillard, Phototransformations of solid pentachlorophenol. Journal of Photochemistry and Photobiology, 119 (1998) 137-142.
20. 浅利 美鈴、高月 紘、酒井 伸一，『廃木材を利用した建築部材（パーティクルボード）製造プロセスにおける化学物質の挙動』，廃棄物学会論文誌, 15 (2004) 139-148.
21. L.F. Lin, W.J. Lee, H.W. Li, M.S. Wang, G.P. Chang-Chie, Characterization and inventory of PCDD/F emissions from coal-fired power plants and other sources in Taiwan. Chemosphere, 68 (2007) 1642-1649.
22. J.C. Hu, M.H. Zheng, W.B. Liu, Z.Q. Nie, C.L. Li, G.R. Liu, K. Xiao, Characterization of polychlorinated dibenzo-p-dioxins and dibenzofurans, dioxin-like polychlorinated biphenyls, and polychlorinated naphthalenes in the environment surrounding secondary copper and aluminum metallurgical facilities in China. Environment Pollution, 193 (2014) 6-12.
23. M.L. Shih, W.J. Lee, T.S. Shih, S.L. Huang, G.P. Chang-Chien, L.C. Wang, P.J. Tsai, Characterization of dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the atmosphere of different workplaces of a sinter plant. Science of the Total Environment, 366 (2006) 197-205.
24. S.J. Chen, W.S. Lee, G.P. Chang-Chien, L.C. Wang, W.J. Lee, J.H. Kao, M.T. Hu, Characterizing polychlorinated dibenzo-p-dioxins and dibenzofurans in the surrounding environment and workplace of a secondary aluminum smelter. Atmospheric. Environment, 38 (2004) 3739-373.
25. C. Zou, J.L. Han, H.Q. Fu, Emissions of PCDD/Fs from steel and secondary nonferrous productions. Procedia Environmental Sciences, 16 (2012) 279-288.
26. W. Loo, Dioxin/furan formation and release in the cement industry. Environmental Toxicology and Pharmacology, 25 (2008) 128-130.
27. M.B. Chang, H.C. Huang, S.S. Tsai, K.H. Chi, G.P. Chang-Chien, Evaluation of the emission characteristics of PCDD/Fs from electric arc furnaces. Chemosphere, 62 (2006) 1761-1773.
28. H.L. Chen, T.S. Shih, P.C. Huang, C.Y. Hsieh, C.C. Lee, Exposure of arc-furnace-plant workers to polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs). Chemosphere, 64 (2006) 666-671.
29. Y.Y. Deng, P.G. Peng, M. Ren, J.Z. Song, W.L. Huang, The winter effect on formation of PCDD/Fs in Guangzhou by vehicles: A tunnel study. Atmospheric Environment, 45 (2011) 2541-2548.
30. M.D. Rey, R. Font, I. Aracil, PCDD/F emissions from light-duty diesel vehicles operated under highway conditions and a diesel-engine based power generator. Journal of Hazardous Materials, 278 (2014) 116-123.
31. M.W. Zhang, S.K. Zhang, Z.Q. Zhang, Z.C. Xu, G.X. Feng, M.Z. Ren, Influence of a municipal solid waste incinerator on ambient air PCDD/F levels: A comparison of running and non-running periods. Science of the Total Environment, 491-492 (2014) 34-41.
32. H.R. Li, J.L. Feng，G.Y. Sheng, S.L. Lu, J.M. Fu, P. Peng, R. Man, The PCDD/F and PBDD/F pollution in the ambient atmosphere of Shanghai, China. Chemosphere, 70 (2008) 576-583.
33. W. Wang, S.T. Qin, Y. Song, Q. Xu, Y.W. Ni, J.P. Chen, X.P. Zhang, Jun Mu, X.H. Zhu, Pollution level and distribution of PCDD/PCDF congeners between vapor phase and particulate phase in winter air of Dalian, China. Journal of Environmental Sciences, 23 (2011) 36-39.
34. Z.Y. Ren, B. Zhang, P. Lu, C. Li, L.R. Gao, M.H. Zheng, Characteristics of air pollution by polychlorinated dibenzo-p-dioxins and dibenzofurans in the typical industrial areas of Tangshan City, China. Journal of Environmental Sciences, 23(2) (2011) .228-235, 2011.
35. L. Ding, Y.M. Li, P. Wang, X.M. Li, Z.S. Zhao, Q.H. Zhang, T. Tuan, G.B. Jiang, Seasonal trend of ambient PCDD/Fs in Tianjin City, northern China using active sampling strategy. Journal of Environmental Sciences, 24(11) (2012) 1966-1971.
36. H.R. Li, L. Zhou, M. Ren, G.Y. Sheng, J.M. Fu, P. Peng, Levels, profiles and gas-particle distribution of atmospheric PCDD/Fs in vehicle parking lots of a South China metropolitan area. Chemosphere, 94 (2014) 128-134.
37. M.M. Rahman, K.H. Kim, R.J.C. Brown, I.S. Bae, C.G. Park, PCDD and PCDF concentrations in a traffic tunnel environment. Science of the Total Environment, 493 (2014) 773-780.
38. H. Kakimoto, H. Oka, Y. Harada, S. Ushijima, A. Toriba, R. Kizu, K. Hayakawa, Comparison of Compositions of Polychlorinated Dibenzo-p-dioxins (PCDDs) Dibenzofurans (PCDFs) in Air and Soil Samples Collected in Ishikawa. Journal of Health Science, 50(1) (2004) 58-65.
39. M.B. Chang, Y.M. Weng, T.Y. Lee, Y.W. Chen, S.H. Chang, K.H. Chi, Sampling and analysis of ambient dioxins in northern Taiwan. Chemosphere, 51 (2003) 1103-1110.
40. 劉敏宏，『重工業都會區污染源排放廢氣及環境介質中戴奧辛/呋喃之特徵』，碩士論文，國立成功大學環境工程研究所，2006。
41. Y.L. Wu, L.F. Lin, L.T. Hsieh, L.C. Wang, G.P. Chang-Chien, Atmospheric dry deposition of polychlorinated dibenzo-p-dioxins and debenzofurans in the vicinity of municipal solid waste incinerators. Journal of Hazardous Materials, 162 (2009) 521-529.
42. M. Ren, P. Peng, S.K. Zhang, L.P. Yu, G. Zhang, B.X. Mai, G.Y. Sheng, J.M. Fu, Atmospheric deposition of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in Guangzhou, China. Atmospheric Environment, 41 (2007) 592-605.
43. K.H. Chi, K.T. Liu, S.H. Chang, M.B. Chang, Atmospheric deposition of PCDD/Fs measured via automated and traditional samplers in Northern Taiwan. Chemosphere, 77 (2009) 1184-1190.
44. H. Oka, H. Kakimoto, Y. Miyata, Y. Yonezawa, A. Niikawa, H. Kyudoh, R. Kizu, K. Hayakawa, Atmospheric Deposition of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) in Kanazawa, Japan. Journal of Health Science, 52(3) (2006) 300-307.
45. L.H. Raun, O. Correa, H. Rifai, M. Suarez, L. Koenig, Statistical investigation of polychlorinated dibenzo-p-dioxins and dibenzofurans in the ambient air of Houston, Texas. Chemosphere, 60 (2005) 973-989.
46. R. Lohmann, P.A. Brunciak, J. Dachs, C.L. Gigliotti, E. Nelson, D.V. Ry, T. Glenn, S.J. Eisenreich, J.L. Joes, K.C. Jones, Processes controlling diurnal variations of PCDD/Fs in the New Jersey coastal atmosphere. Atmospheric Environment, 37 (2003) 959-969.
47. M. Ragazzi, E.C. Rada, M. Marconi, A. Chiste, S. Fedrizzi, G. Segatta, M. Schiavon, G. Ionescu, Characterization of the PCDD/F in the Province of Trento. Energy Procedia, 50 (2014) 945-952.
48. Y. Moussaoui, L. Tuduri, Y. Kerchich, B.Y. Meklati, G. Eppe, Atmospheric concentrations of PCDD/Fs, dl-PCBs and some pesticides in northern Algeria using passive air sampling. Chemosphere, 88 (2012) 270-277.
49. E. Abad, K. Martinez, L. Gustems, R. Gomez, X. Guinart, I. Hernandez, J. Rivera, Ten years measuring PCDDs/PCDFs in ambient air in Catalonia (Spain). Chemosphere, 67 (2007) 1709-1714.
50. 賴沛君、鄭曼婷，『應用CMB受體模式分析懸浮微粒高污染事件之研究』，碩士論文，國立中興大學環境工程研究所，2004。
51. 邱嘉斌、鄭曼婷，『應用CMB受體模式分析懸浮微粒高污染事件之研究』，博士論文，國立中興大學環境工程研究所，2005。
52. 葉振元、謝連德，『以CMB受體模式解析高屏地區交通路口PM上水溶性離子之研究』，碩士論文，屏東科技大學環境工程與科學系所，2010。
53. P. Pant, J.X. Yin, R.M. Harison, Sensitivity of a Chemical Mass Balance model to different molecular marker traffic source profiles. Atmospheric Environment, 82 (2014) 238-249.
54. J. Heo, M. Dulger, M.R. Olson, J.E. McGinnis, B.R. Shelton, A. Matsunaga, C. Sioutas, J.J. Schauer, Source apportionments of PM2.5 organic carbon using molecular marker Positive Matrix Factorization and comparison of results from different receptor models. Atmospheric Environment, 73 (2013) 51-61.
55. S. Hasheminassab, N. Daher, J.J. Schauer, C. Sioutas, Source apportionment and organic compound characterization of ambient ultrafine particulate matter (PM) in the Los Angeles Basin. Atmospheric Environment, 79 (2013) 529-539.
56. A. Colombo, E. Benfenati, S.G. Bugatti, M. Lodi, A. Mariani, L. Musmeci, G. Rotella, V. Senese, G. Ziemacki, R. Fanelli, PCDD/Fs and PCBs in ambient air in a highly industrialized city in Northern Italy. Chemosphere, 90 (2013) 2352-2357.
57. M.W. Zhang, S.K. Zhang, Z.Q. Zhang, Z.C. Xu, G.X. Feng, M.Z. Ren, Influence of a municipal solid waste incinerator on ambient air PCDD/F levels: A comparison of running and non-running periods. Science of the Total Environment, 491-492 (2014) 34-41.
58. T.Y. Wu, Y.C. Lin, Y.M. Chen, G.P. Chang-Chien, Impacts of dust storms on PCDD/Fs and regulated harmful matter in a basin area. Atmospheric Research, 97 (2010) 279-293.
59. 楊智閔、鄭芳怡，『探討台灣地區在春季期間經長程傳輸所觀測之一氧化碳濃度與綜觀天氣之關係』，碩士論文，國立中央大學大氣物理研究所，2012。
60. 曹耀文、陳宏瑜，『台灣北部沿岸區域乾沈降中無機性與有機性氮物種統計檢定分析與通量之研究』，碩士論文，國立臺灣海洋大學海洋 環境資訊系，2010。
61. 黃堯聖、陳世裕、江鴻龍，『大氣懸浮微粒化學組成及來源推估』，碩士論文，輔英科技大學環境工程與科學系，2006。
62. M. Sadys, C.A. Skjoth, R. Kennedy, Back-trajectories show export of airborne fungal spores (Ganoderma sp.) from forests to agricultural and urban areas in England. Atmospheric Environment, 84 (2014) 88-99.
63. R. Betha, Z. Zhang, R. Balasubramanian, Influence of trans-boundary biomass burning impacted air masses on submicron particle number concentrations and size distributions. Atmospheric Environment, 92 (2014) 9-18.
64. L. Ding, Y.M. Li, P. Wang, X.M. Li, Z.S. Zhao, Q.H. Zhang, T. Tuan, G.B. Jiang, Seasonal trend of ambient PCDD/Fs in Tianjin City, northern China using active sampling strategy. Journal of Environmental Sciences, 24(11) (2012) 1966-1971.
65. N.T. Thuan, K.H. Chi, S.H. Wang, M.B. Chang, N.H. Lin, G.R. Sheu, C.M. Peng, Atmospheric PCDD/F measurement in Taiwan and Southeast Asia during Dongsha Experiment. Atmospheric Environment, 78 (2013) 195-202.
66. E.S.C. Kwok, R. Atkinson, J. Arey, Rate constants for the gas-phase reactions of the OH radical with dichlorophenyl, 1-chlorobenzo-p-dioxin, 1,2-dimethoxybenzene and diphenyl ether: estimate of OH radical rate constants for PCBs, PCDDs and PCDFs. Environmental Science & Technology, 29 (1995) 1591-1598.
67. G. Mckay, Dioxin characterisation, formation and minimisation during municipal solid waste (MSW) incineration: review. Chemical Engineering Journal, 86 (2002) 343-3
68. W. Moche, G. Thanner, PCDD/F-emissions from coal combustion in small residential plants. Organohalogen Comp, 36 (1998) 329-332.