簡易檢索 / 詳目顯示

研究生: 郁揆民
Yu, Kuei-Min
論文名稱: 含戴奧辛/呋喃飛灰處理廠對周遭環境之影響評估
Environmental Impact Assessment of A Polychlorinated Dibenzo-p-dioxin and Dibenzofuran Contained Fly Ash Treatment Plant
指導教授: 李文智
Lee, Wen-Jhy
共同指導教授: 吳義林
Wu, Yee-Lin
學位類別: 博士
Doctor
系所名稱: 工學院 - 環境工程學系
Department of Environmental Engineering
論文出版年: 2010
畢業學年度: 98
語文別: 英文
論文頁數: 85
中文關鍵詞: 戴奧辛呋喃電弧爐飛灰點源排放面源逸散排放因子
外文關鍵詞: PCDD/Fs, electric-arc furnace-dust, stack emission, fugitive emission, emission factor
相關次數: 點閱:118下載:3
分享至:
查詢本校圖書館目錄 查詢臺灣博碩士論文知識加值系統 勘誤回報
  • 戴奧辛類化合物為環境中具有嚴重危害之化合物之一,可藉由工業熱處理程序產生並排放至大氣中造成環境衝擊。電弧爐煉鋼程序亦適合戴奧辛之形成,其煙道氣飛灰中常含有大量戴奧辛及重金屬,為處理電弧爐飛灰並回收其中重金屬而設立之電弧爐飛灰處理廠利用高溫旋轉窯進行重金屬回收,因處理高戴奧辛含量之飛灰,同時也是適合戴奧辛生成之熱處理程序,故為主要之戴奧辛污染源。本研究評估台灣地區一電弧飛灰處理廠對鄰近地區環境戴奧辛之衝擊。
    本研究之內容主要分為二部分:一、分析電弧爐飛灰處理廠大氣中粒狀戴奧辛特徵,藉以評估難以監測及防治之面源逸散戴奧辛特徵,結果用以進行第二部分之模式推估;二、對該廠之煙道戴奧辛濃度進行監測,並求得點源排放速率,同時以廠內大氣戴奧辛濃度配合模式推估面源之戴奧辛逸散速率,再利用模式推估目前之戴奧辛排放、逸散速率對鄰近地區之影響。
    第一部分之研究結果顯示:電弧爐飛灰處理廠之面源逸散戴奧辛多分佈於容易沉降之粗顆粒,屬於易隨大氣擴散之細顆粒在49%以下,而其他廠外污染源排放之戴奧辛54%以上分佈於細顆粒,顯示廠內逸散之戴奧辛隨大氣傳輸至其他地區可能性較低。
    第二部分之研究結果顯示:面源逸散戴奧辛量之速率及排放因子均高於點源排放,故點源排放之戴奧辛經空氣污染處理設備後可確實控制。以本研究求得之點源排放及面源逸散速率推估該電弧爐飛灰處理廠對鄰近地區大氣中戴奧辛之貢獻量,發現點源排放之戴奧辛濃度僅0.27 fg I-TEQ/Nm3,面源僅3.3 fg I-TEQ/Nm3,與鄰近地區大氣戴奧辛濃度實測值相較,該廠總戴奧辛排放對鄰近地區大氣戴奧辛濃度之貢獻低於10%。
    由本研究之實驗結果顯示,該電弧爐飛灰處理廠面源逸散之戴奧辛量可能較點源排放量高,顯示面源逸散戴奧辛應視為與點源排放同樣重要之監測項目,作為環境衝擊評估之參考。該廠對鄰近地區大氣戴奧辛濃度之貢獻並不顯著,且點源排放、大氣戴奧辛濃度及鄰近地區之大氣戴奧辛濃度均合符國內外法規之規範。面源逸散戴奧辛之懸浮微粒為環境中較易沉降之粗粒徑微粒。

    The dioxin-like compounds are one of the most hazardous material groups in the world. Electric-arc furnace-dust treatment plant (EAFDTP) has been defined as the major PCDD/F source in many countries due to its raw material containing huge amount of PCDD/Fs and chloride and its thermal process provide an environment for PCDD/F formation. The major objective of this study is to evaluate the PCDD/F environmental impact of a selected EAFDTP in Taiwan.
    The research is mainly contained two parts: the first part is to investigate the size distributions of particulate, PCDD/F mass and toxic equivalent (TEQ) in the ambient air of two sampling sites near fugitive emission sources in the EAFDTP; and the second part is set out to investigate emissions of PCDD/Fs from both the stack (i.e., point source) and plant fugitives (i.e., area source) of an EAFDTP and their impact to the vicinity environments.
    The results of the first part show that the fugitive sources in EAFDTP less than 49% of total PCDD/Fs and toxic equivalents (TEQs) were found to be associated with fine particles, more than 54% of total PCDD/Fs and TEQs were correlated with fine particles from outside-plant emission sources. These reveal that fugitive PCDD/Fs from EAFDTP would stay in the plant rather than dispersion in the atmosphere.
    The results of the second part show that both the PCDD/F fugitive rate and factor of EAFDTP were higher than stack emission, which suggested that PCDD/Fs in stack flue gas could be control by air pollution control devices (APCDs). Base on the stack emission rate and fugitive rate of EAFDTP those were monitered and estimated in this study, the atmospheric PCDD/F impacts in the vicinity of EAFDTP were assessed. It has been found that the contribution of stack emission was lower than 0.27 fg I-TEQ/Nm3, and was lower than 3.3 fg I-TEQ/Nm3 for fugitive emission. Comparing to the practical atmospheric PCDD/F concentration in the vincinity, total PCDD/F contribution of EAFDTP was less than 10%.
    The study illustrates that the particle-bound PCDD/Fs from fugitive emission sources of EAFDTP concentrated on coarse particulates may help PCDD/Fs to deposit to the ground level. The MMDo values of PCDD/F TEQs that came from other sources (1.08, 1.86 μm) outside of the EAFDTP were smaller than those from EAFDTP (2.77, 11.3 μm), and appare to impact humans and the environment significantly. The mean emission rate of the area source (2590 ng I-TEQ/hr) was greater than that of point source (2360 ng I-TEQ/hr). Our result indicates that the area source contributed more than 50% of the total PCDD/Fs emission from the EAFDTP to the ambient atmospheric environments.

    中文摘要 I ABSTRACT III Acknowledgement /誌謝 VI Contents/總目錄 VII List of Tables/表目錄 X List of Figures/圖目錄 XI Chapter 1 Introduction 13 1.1 Goal and Specific Aims 13 1.2 Background and Significance 13 1.3 Overview 14 Chapter 2 Literature Survey 16 2.1 Characteristics of PCDD/Fs 16 2.2 Mechanisms of PCDD/F Formation 18 2.3 Particle Size Distribution of PCDD/F 18 2.4 Electrical Arc Furnace 19 2.5 Electrical Arc Furnace Dust Treatment 20 Chapter 3 Materials and Methods 22 3.1 The Procedure of the Experiments 22 3.2 Particle Size Distribution Sampling 23 3.2.1 Sampling Sites and Periods 23 3.2.2 Sampling Method 25 3.2.2.1 MOUDI 25 3.2.2.2 NRI 27 3.2.2.3 Combine the size ranges of MOUDI and NRI 29 3.2.3 Parameters for Describing Particle Size Distributions 29 3.2.4 Meteorology for Particle Size Distribution Sampling 30 3.3 PCDD/F Emission Factors 32 3.3.1 Sampling Period and the Corresponding Meteorology 32 3.3.2 Sampling Sites 32 3.3.3 Sampling Method 36 3.3.3.1 Atmospheric PCDD/Fs 36 3.3.3.2 Stack Emits PCDD/Fs 39 3.4 PCDD/F Analysis 39 3.4.1 Instruments and Conditions 39 3.4.2 Quality Assurance and Quality Control (QA/QC) 40 3.5 Emission Factor 41 3.5.1 The Emission Factor of Point Source 41 3.5.2 The Emission Factor of Area Source 41 3.6 PCDD/F Contribution of EAFDTP in the Vincinity 42 Chapter 4 Results and Discussion 43 4.1 Atmospheric Particle Size Distribution 43 4.1.1 Particle Size Distribution of Total Particle Mass 43 4.1.2 Concentration of PCDD/Fs with Particle Size 46 4.1.3 Particle Size Distribution of Total PCDD/Fs and Total PCDD/F-TEQs 50 4.1.4 Cumulative Fraction of Particle Size Distribution 53 4.1.5 MMD and σg 55 4.2 PCDD/F Emission Factors of EAFDTP 60 4.2.1 PCDD/F Concentrations of the Site P, Site U and Site D 60 4.2.2 ISCST3 64 4.2.3 Emission of PCDD/Fs from the Point- and Area-Sources 66 4.2.4 Contributions of Point- and Area-Sources to the Vincinity Atmospheric Environments 68 Chapter 5 Conclusion and Suggestions 71 5.1 Conclusions 71 5.2 Suggestions 72 References 74 Resume (自述) 82

    Bidleman T F. Atmospheric processes - wet and dry deposition of organic-compounds are controlled by their vapor particle partitioning. Environ. Sci. Technol., Vol. 22, No. 4, pp. 361-367, 1988.

    Brown D J, Chu M, Van Overmeire I, Chu A and Clark G C. Determination of rep values for the calux® bioassay and comparison to the who tef values. Organohalogen Compounds, Vol. 53, No., pp. 211-214, 2001.

    Chang M B, Huang H C, Tsai S S, Chi K H and Chang-Chien G P. Evaluation of the emission characteristics of pcdd/fs from electric are furnaces. Chemosphere, Vol. 62, No. 11, pp. 1761-1773, 2006.

    Chao M R, Hu C W, Ma H W, Chang-Chien G P, Lee W J, Chang L W and Wu K Y. Size distribution of particle-bound polychlorinated dibenzo-p-dioxins and dibenzofurans in the ambient air of a municipal incinerator. Atmos. Environ., Vol. 37, No. 35, pp. 4945-4954, 2003.

    Chen C K, Lin C, Lin Y C, Wang L C and Chang-Chien G P. Polychlorinated dibenzo-p-dioxins/dibenzofuran mass distribution in both start-up and normal condition in the whole municipal solid waste incinerator. J. Hazard. Mater., Vol. 160, No. 1, pp. 37-44, 2008.

    Chi K H, Chang S H and Chang M B. Characteristics of pcdd/f distributions in vapor and solid phases and emissions from the waelz process. Environ. Sci. Technol., Vol. 40, No. 6, pp. 1770-1775, 2006.

    Dickson L C, Lenoir D and Hutzinger O. Surface-catalyzed formation of chlorinated dibenzodioxins and dibenzofurans during incineration. Chemosphere, Vol. 19, No. 1-6, pp. 277-282, 1989.

    Dyke P H and Stratford J. Changes to the tef schemes can have significant impacts on regulation and management of pcdd/f and pcb. Chemosphere, Vol. 47, No. 2, pp. 103-116, 2002.

    Everaert K and Baeyens J. The formation and emission of dioxins in large scale thermal processes. Chemosphere, Vol. 46, No. 3, pp. 439-448, 2002.

    Gass H C, Werner C, Sunderhauf W and Meisser J. Dioxin emission after failure in activated carbon injection at a steel plant. 25th International Symposium on Halogenated Environmental Organic Pollutants and Persistent Organics Pollutants. 2005.

    Hutzinger O, Blumich M J, Vanderberg M and Olie K. Sourcesand fate of pcdds and pcdfs - an overview. Chemosphere, Vol. 14, No. 6-7, pp. 581-600, 1985.

    Japanese Ministry of the Environment. The environmental monitoring report on the persistent organic pollutants (pops) in Japan. Tokyo. 39, 2002.

    Kao J H, Chen K S, Chang-Chien G P and Chou I C. Emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans from various stationary sources. Aerosol Air Qual. Res., Vol. 6, No. 2, pp. 170-179, 2006.

    Kouimtzis T, Samara C, Voutsa D, Balafoutis C and Muller L. Pcdd/fs and pcbs in airborne particulate matter of the greater thessaloniki area, n. Greece. Chemosphere, Vol. 47, No. 2, pp. 193-205, 2002.

    Kurokawa Y, Matsueda T, Nakamura M, Takada S and Fukamachi K. Characterization of non-ortho coplanar pcbs, polychlorinated dibenzo-p-dioxins and dibenzofurans in the atmosphere. Chemosphere, Vol. 32, No. 3, pp. 491-500, 1996.

    Lee R G M and Jones K C. Gas-particle partitioning of atmospheric pcdd/fs: Measurements and observations on modeling. Environ. Sci. Technol., Vol. 33, No. 20, pp. 3596-3604, 1999.

    Lee W J, Liow M C, Hsieh L T, Chen T J H and Tsai P J. Impact of polycyclic aromatic hydrocarbon emissions from medical waste incinerators on the urban atmosphere. J. Air Waste Manage. Assoc., Vol. 53, No. 9, pp. 1149-1157, 2003.

    Lee W J, Shih S I, Li H W, Lin L F, Yu K M, Lu K, Wang L C, Chang-Chien G P, Fang K and Lin M. Assessment of polychlorinated dibenzo-p-dioxins and dibenzofurans contribution from different media to surrounding duck farms. J. Hazard. Mater., Vol. 163, No. 2-3, pp. 1185-1193, 2009.

    Lee W J, Su C C, Sheu H L, Fan Y C, Chao H R and Fang G C. Monitoring and modeling of pcb dry deposition in urban area. J. Hazard. Mater., Vol. 49, No. 1, pp. 57-88, 1996.

    Li H W, Lee W J, Tsai P J, Mou J L, Chang-Chien G P and Yang K T. A novel method to enhance polychlorinated dibenzo-p-dioxins and dibenzofurans removal by adding bio-solution in eaf dust treatment plant. J. Hazard. Mater., Vol. 150, No. 1, pp. 83-91, 2008.

    Li H W, Wu Y L, Lee W J and Chang-Chien G P. Fate of polychlorinated dibenzo-p-dioxins and dibenzofurans in a fly ash treatment plant. J. Air Waste Manage. Assoc., Vol. 57, No. 9, pp. 1024-1031, 2007.

    Lin L F, Lee W J, Hsing-Wang L B, Wang M S and Chang-Chien G P. Characterization and inventory of pcdd/f emissions from coal-fired power plants and other sources in taiwan. Chemosphere, Vol. 68, No. 9, pp. 1642-1649, 2007.

    Lohmann R and Jones K C. Dioxins and furans in air and deposition: A review of levels, behaviour and processes. Sci. Total Environ., Vol. 219, No. 1, pp. 53-81, 1998.

    Lorber M, Pinsky P, Gehring P, Braverman C, Winters D and Sovocool W. Relationships between dioxins in soil, air, ash, and emissions from a municipal solid waste incinerator emitting large amounts of dioxins. Chemosphere, Vol. 37, No. 9-12, pp. 2173-2197, 1998.

    Lustenhouwer J W A, Olie K and Hutzinger O. Chlorinated dibenzo-p-dioxins and related-compounds in incinerator effluents - a review of measurements and mechanisms of formation. Chemosphere, Vol. 9, No. 7-8, pp. 501-522, 1980.

    Mager K, Meurer U and Wirling J. Minimizing dioxin and furan emissions during zinc dust recycle by the waelz process. JOM-J. Miner. Met. Mater. Soc., Vol. 55, No. 8, pp. 20-25, 2003.

    Mandal P K. Dioxin: A review of its environmental effects and its aryl hydrocarbon receptor biology. Journal of Comparative Physiology B: Biochemical, Systemic, and Environmental Physiology, Vol. 175, No. 4, pp. 221-230, 2005.

    Mi H H, Chiang C F, Lai C C, Wang L C and Yang H H. Comparison of pah emissions from a municipal waste incinerator and mobile sources. Aerosol Air Qual. Res., Vol. 1, No. 1, pp. 83-90, 2001.

    Noll K E, Pontius A, Frey R and Gould M. Comparison of atmospheric coarse particles at an urban and non-urban site. Atmos. Environ., Vol. 19, No. 11, pp. 1931-1943, 1985.

    Noll K E, Yuen P F and Fang K Y P. Atmospheric coarse particulate concentrations and dry deposition fluxes for 10 metals in 2 urban environments. Atmos. Environ. Part A, Vol. 24, No. 4, pp. 903-908, 1990.

    Oberdorster G, Ferin J and Lehnert B E. Correlation between particle-size, in-vivo particle persistence, and lung injury. Environ. Health Perspect., Vol. 102, No., pp. 173-179, 1994.

    Olie K, Vermeulen P L and Hutzinger O. Chloro di benzo-p-dioxins and chloro di benzo furans are trace components of fly ash and flue gas of some municipal incinerators in the netherlands. Chemosphere, Vol. 6, No. 8, pp. 455-459, 1977.

    Quass U, Fermann M W and Broker G (2000). The european dioxin emission inventory stage ii. 1: 27.

    Schlesinger R B, Kunzli N, Hidy G M, Gotschi T and Jerrett M. The health relevance of ambient particulate matter characteristics: Coherence of toxicological and epidemiological inferences. Inhal. Toxicol., Vol. 18, No. 2, pp. 95-125, 2006.

    Sheu H L, Lee W J, Lin S J, Fang G C, Chang H C and You W C. Particle-bound pah content in ambient air. Environ. Pollut., Vol. 96, No. 3, pp. 369-382, 1997.

    Stewart B W and Kleihues P. World cancer report. Lyon, Pages, 2003.

    Tuppurainen K A, Ruokojarvi P H, Asikainen A H, Aatamila M and Ruuskanen J. Chlorophenols, as precursors of pcdd/fs in incineration processes: Correlations, pls modeling, and reaction mechanisms. Environ. Sci. Technol., Vol. 34, No. 23, pp. 4958-4962, 2000.

    Van den Berg M, Birnbaum L S, Denison M, De Vito M, Farland W, Feeley M, Fiedler H, Hakansson H, Hanberg A, Haws L, Rose M, Safe S, Schrenk D, Tohyama C, Tritscher A, Tuomisto J, Tysklind M, Walker N and Peterson R E. The 2005 world health organization reevaluation of human and mammalian toxic equivalency factors for dioxins and dioxin-like compounds. Toxicol. Sci., Vol. 93, No. 2, pp. 223-241, 2006.

    van Leeuwen F X R, Feeley M, Schrenk D, Larsen J C, Farland W and Younes M. Dioxins: Who's tolerable daily intake (tdi) revisited. Chemosphere, Vol. 40, No. 9-11, pp. 1095-1101, 2000.

    Wang J B, Wang M-S, Wu E M-Y, Chang-Chien G-P and Lai Y-C. Approaches adopted to assess environmental impacts of pcdd/f emissions from a municipal solid waste incinerator. J. Hazard. Mater., Vol. 152, No. 3, pp. 968-975, 2008.

    Wang L C, Lee W J, Lee W S, Chang-Chien G P and Tsai P J. Effect of chlorine content in feeding wastes of incineration on the emission of polychlorinated dibenzo-p-dioxins/dibenzofurans. Sci. Total Environ., Vol. 302, No. 1-3, pp. 185-198, 2003.

    Wang Y F, Chao H R, Wu C H, Wang L C, Chang-Chien G P, Yang H H, Lin D Y and Tsou T C. Emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans from a heavy oil-fueled power plant in northern taiwan. J. Hazard. Mater., Vol. 163, No. 1, pp. 266-272, 2009.

    Yang H-H, Lee W-J, Chen S-J and Lai S-O. Pah emission from various industrial stacks. J. Hazard. Mater., Vol. 60, No. 2, pp. 159-174, 1998.

    Yang H H, Chiang C F, Lee W J, Hwang K P and Wu E M Y. Size distribution and dry deposition of road dust pahs. Environ. Int., Vol. 25, No. 5, pp. 585-597, 1999.

    Yu B W, Moon Y H, Kim M K, Kyoung J D and Chang Y S. Inventory study of pcdd/fs for metal industries in south korea. Federal Environmental Agency, Vienna, AUTRICHE, 2003.

    Yu K M, Wu Y L, Fang K and Lin M. Particle size distribution of polychlorinated dibenzo-p-dioxins and dibenzofurans in the ambient air of an electric-arc furnace-dust treatment plant. Environ. Eng. Sci., Vol. 26, No. 12, pp. 1713-1723, 2009.

    下載圖示 校內:2013-08-06公開
    校外:2013-08-06公開
    QR CODE