| 研究生: |
鄭凱倫 Cheng, Kai-Lun |
|---|---|
| 論文名稱: |
台灣北部地區大氣中戴奧辛/口夫喃之氣固相分佈及乾沉降研究 Both Phase Distributions and Dry Deposition of Polychlorinated Dibenzo-p-dioxins, Dibenzofurans in the Ambient Air of Northern Taiwan |
| 指導教授: |
李文智
Lee, Wen-Jhy |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 環境工程學系 Department of Environmental Engineering |
| 論文出版年: | 2013 |
| 畢業學年度: | 101 |
| 語文別: | 英文 |
| 論文頁數: | 77 |
| 中文關鍵詞: | 戴奧辛/呋喃 、焚化廠 、大氣濃度 、氣固相分佈 、乾沉降 |
| 外文關鍵詞: | Polychlorinated Dibenzo-p-dioxins, Dibenzofurans, municipal solid waste incinerators, atmospheric concentration, gas-particle partition, dry deposition |
| 相關次數: | 點閱:118 下載:0 |
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本研究目的為了解台灣北部焚化廠周界大氣中PCDD/Fs之濃度、氣固相分佈特徵以及乾沉降通量,分別自2006年至2011年針對台灣北部三座焚化廠周界地區進行大氣PCDD/Fs濃度之採樣調查,每座焚化廠附近皆選取7處作為採樣點,一次採樣共計21個空氣樣品進行17種PCDD/Fs異構物分析。
從特徵剖面I-TEQ固相濃度來看,以2,3,4,7,8-PeCDF所占比例最高,其次為1,2,3,4,7,8-HxCDF及 1,2,3,6,7,8-HxCDF;若以特徵剖面I-TEQ氣相濃度來看,亦以2,3,4,7,8-PeCDF所佔比例為最高,其次為 2,3,7,8-TeCDD/F及 1,2,3,4,7,8-CDD。進一步研究大氣中氣固相濃度所佔總PCDD/Fs之I-TEQ濃度之比例,發現固相濃度所佔比例以一月(46.7%)、二月(45.0%)及三月(45.6%)為最高,而氣相濃度所佔比例以六月 (87.6%)及八月(87.4%)所佔比例為最高。由2006年至2011年,六年間固相濃度所佔總PCDD/Fs-I-TEQ濃度比例為25.8%至32.0%(平均28.1%),而氣相濃度所佔總PCDD/Fs-I-TEQ濃度比例則為68.0%至74.2%(平均71.2%)
乾沉降通量部分,PCDD/Fs-I-TEQ乾沉降均以粒狀物相沉降為主,所佔比例從87.0% 至 98.3%,平均 94.2%。模擬之逐月PCDD/Fs-I-TEQ乾沉降通量範圍為0.102 ng-I-TEQ/m2-month (三月)至0.307 ng-I-TEQ/m2-month (六月);模擬之逐年PCDD/Fs-I-TEQ乾沉降通量範圍為1.352 ng-I-TEQ/m2-year 至 2.766 ng-I-TEQ/m2-year,其中2009年及20111年有顯著較低之乾沉降通量,可能由於相對較低之PCDD/Fs採樣濃度所導致。平均年乾沉降速度為0.403cm/s至0.506cm/s,無顯著差異之可能原因為六年間之溫度及TSP濃度變化並不大。此研究提供有關大氣中PCDD/Fs行為之探討,可供未來PCDD/Fs相關控制政策制定上之參考。
The objectives of this study were to know the concentration, gas-particle partitioning properties, and dry deposition process of PCDD/Fs in the ambient air in northern Taiwan. During each sampling period from 2006 to 2011, 21 sampling sites, with maximum ground concentration of PCDD/Fs from the emission of each MSWI found by ISCST model, near three municipal solid waste incinerators located in northern Taiwan were selected. Air samples were analyzed for specific 17 PCDD/F congeners, and the protocol for QA/QC is strictly followed.
From congener profiles of PCDD/Fs-I-TEQ in particle phase, the 2,3,4,7,8-PeCDF was the most predominant congener and follow by 1,2,3,4,7,8-HxCDF and 1,2,3,6,7,8-HxCDF. For PCDD/Fs-I-TEQ in gas phase, the 2,3,4,7,8-PeCDF was most dominant one and followed by 2,3,7,8-TeCDD/F and 1,2,3,4,7,8-CDD. For the gas-particle partitioning properties of total PCDD/Fs-I-TEQ, the highest percentage of particle phase occurred in January (46.7%), followed by February (45.0%) and March (45.6%), and the highest percentage of gas phase occurred in July (87.6%), followed by August (87.4%). For the phase distributions of total PCDD/Fs-I-TEQ in six years, the percentage of particle phase ranged from 25.8% to 32.0%, with an average of 28.1%, and the percentage of gas phase ranged from 68.0% to 74.2%, with an average of 71.2%. There was no significant difference among each year.
Mean fraction of PCDD/Fs-I-TEQ dry deposition flux contributed by the particle phase were between 87.0% and 98.3%, and averaged 94.2%. The above results displayed that the particulates is the predominant factor controlling the PCDD/F dry deposition flux in the atmosphere. Modeled mean monthly dry deposition of PCDD/Fs-I-TEQ ranged from 0.102 (in March) to 0.307 ng-I-TEQ/m2-month (in June), probably due to the higher TSP concentration in March and fewer sunny days in summer.
Modeled yearly mean dry deposition of PCDD/Fs-I-TEQ ranged from 1.352 to 2.766 ng-I-TEQ/m2-year, with the significantly lower value in 2009 and 2011, may because of relatively lower PCDD/Fs concentrations. Mean yearly dry deposition velocities of PCDD/Fs-I-TEQ in six years were 0.403 - 0.506 cm/s. Both temperature and TSP concentration were similar during 2006-2011, therefore, the dry deposition velocity in each year was very close. This study provides useful information for looking more inside on the behavior of PCDD/Fs in the ambient air, which is a great benefit for establishing good strategy for the PCDD/Fs control.
Ahlborg, U. G., Brouwer, A., Fingerhut, M. A., Jacobson, J. L., Jacobson, S. W., Kennedy, S. W., Kettrup, A. A. F., Koeman, J. H., Poiger, H., Rappe, C., Safe, S. H., Seegal, R. F., Tuomisto, J. and Vandenberg, M. (1992). Impact of Polychlorinated Dibenzo-P-Dioxins, Dibenzofurans, and Biphenyls on Human and Environmental-Health, with Special Emphasis on Application of the Toxic Equivalency Factor Concept. Eur. J. Pharmacol.-Environ. Toxicol. Pharmacol. Sect. 228:179-199.
Birnbaum, L. S. (1994). Endocrine Effects of Prenatal Exposure to Pcbs, Dioxins, and Other Xenobiotics - Implications for Policy and Future-Research. Environ. Health Perspect. 102:676-679.
Breivik, K., Alcock, R., Li, Y. F., Bailey, R. E., Fiedler, H. and Pacyna, J. M. (2004). Primary Sources of Selected Pops: Regional and Global Scale Emission Inventories. Environmental Pollution 128:3-16.
Caserini, S. and Monguzzi, A. M. (2002). PCDD/Fs Emissions Inventory in the Lombardy Region: Results and Uncertainties. Chemosphere 48:779-786.
Chang, M. B., Weng, Y. M., Lee, T. Y., Chen, Y. W., Chang, S. H. and Chi, K. H. (2003). Sampling and Analysis of Ambient Dioxins in Northern Taiwan. Chemosphere 51:1103-1110.
Chao, M. R., Hu, C. W., Chen, Y. L., Chang-Chien, G. P., Lee, W. J., Chang, L. W., Lee, W. S. and Wu, K. Y. (2004). Approaching Gas-Particle Partitioning Equilibrium of Atmospheric PCDD/Fs with Increasing Distance from an Incinerator: Measurements and Observations on Modeling. Atmos. Environ. 38:1501-1510.
Chen, C.-M. (2004). The Emission Inventory of PCDD/PCDF in Taiwan. Chemosphere 54:1413-1420.
Coleman, P. J., Lee, R. G. M., Alcock, R. E. and Jones, K. C. (1997). Observations on Pah, PCB, and PCDD/F Trends in Uk Urban Air, 1991-1995. Environ. Sci. Technol. 31:2120-2124.
Cristale, J., Quintana, J., Chaler, R., Ventura, F. and Lacorte, S. (2012). Gas Chromatography/Mass Spectrometry Comprehensive Analysis of Organophosphorus, Brominated Flame Retardants, by-Products and Formulation Intermediates in Water. J. Chromatogr. A 1241:1-12.
Czuczwa, J. M. and Hites, R. A. (1986). Airborne Dioxins and Dibenzofurans - Sources and Fates. Environ. Sci. Technol. 20:195-200.
Donnelly, J. R., Munslow, W. D., Mitchum, R. K. and Sovocool, G. W. (1987). Correlation of Structure with Retention Index for Chlorinated Dibenzo-P-Dioxins. J. Chromatogr. A 392:51-63.
Eduljee, G. H. and Dyke, P. (1996). An Updated Inventory of Potential PCDD and PCDF Emission Sources in the Uk. Sci. Total Environ. 177:303-321.
Eitzer, B. D. and Hites, R. A. (1989). Atmospheric Transport and Deposition of Polychlorinated Dibenzo-Para-Dioxins and Dibenzofurans. Environ. Sci. Technol. 23:1396-1401.
Eitzer, B. D. and Hites, R. A. (1988). Vapor-Pressures of Chlorinated Dioxins and Dibenzofurans. Environ. Sci. Technol. 22:1362-1364.
Everaert, K. and Baeyens, J. (2002). The Formation and Emission of Dioxins in Large Scale Thermal Processes. Chemosphere 46:439-448.
Fiedler, H. (1996). Sources of PCDD/PCDF and Impact on the Environment. Chemosphere 32:55-64.
Huang, C. J., Chen, K. S., Lai, Y. C., Wang, L. C. and Chang-Chien, G. P. (2011). Characterization of Atmospheric Dry Deposition of Polychlorinated Dibenzo-P-Dioxins/Dibenzofuran in a Rural Area of Taiwan. Aerosol Air Qual. Res. 11:448-459.
Huang, H. and Buekens, A. (1995). On the Mechanisms of Dioxin Formation in Combustion Processes. Chemosphere 31:4099-4117.
Hung, H., Blanchard, P., Poole, G., Thibert, B. and Chiu, C. H. (2002). Measurement of Particle-Bound Polychlorinated Dibenzo-P-Dioxins and Dibenzofurans (PCDD/Fs) in Arctic Air at Alert, Nunavut, Canada. Atmos. Environ. 36:1041-1050.
Hutzinger, O. and Fiedler, H. (1989). Sources and Emissions of PCDD/PCDF. Chemosphere 18:23-32.
Ikonomou, M. G., Rayne, S. and Addison, R. F. (2002). Exponential Increases of the Brominated Flame Retardants, Polybrominated Diphenyl Ethers, in the Canadian Arctic from 1981 to 2000. Environ. Sci. Technol. 36:1886-1892.
Jurado, E., Jaward, F. M., Lohmann, R., Jones, K. C., Simo, R. and Dachs, J. (2004). Atmospheric Dry Deposition of Persistent Organic Pollutants to the Atlantic and Inferences for the Global Oceans. Environ. Sci. Technol. 38:5505-5513.
Kao, W. Y., Ma, H. W. and Chang-Chien, G. P. (2011). Evaluation of Incremental Population and Individual Carcinogenic Risks of PCDD/Fs from Steel and Iron Industry in Taiwan by a Site-Specific Health Risk Assessment Method. Aerosol Air Qual. Res. 11:716-731.
Karademir, A. (2004). Health Risk Assessment of PCDD/F Emissions from a Hazardous and Medical Waste Incinerator in Turkey. Environment International 30:1027-1038.
Kutz, F. W., Barnes, D. G., Bottimore, D. P., Greim, H. and Bretthauer, E. W. (1990). The International Toxicity Equivalency Factor (I-TEF) Method of Risk Assessment for Complex Mixtures of Dioxins and Related Compounds. Chemosphere 20:751-757.
Lee, W. J., Su, C. C., Sheu, H. L., Fan, Y. C., Chao, H. R. and Fang, G. C. (1996). Monitoring and Modeling of PCB Dry Deposition in Urban Area. Journal of Hazardous Materials 49:57-88.
Lin, L. F., Shih, S. I., Su, J. W., Shih, M. L., Lin, K. C., Wang, L. C. and Chang-Chien, G. P. (2010a). Dry and Wet Deposition of Polychlorinated Dibenzo-P-Dioxins and Dibenzofurans on the Drinking Water Treatment Plant. Aerosol Air Qual. Res. 10:231-244.
Lin, W. Y., Wu, Y. L., Tu, L. K., Wang, L. C. and Lu, X. (2010b). The Emission and Distribution of PCDD/Fs in Municipal Solid Waste Incinerators and Coal-Fired Power Plant. Aerosol Air Qual. Res. 10:519-532.
Lin, Y. S., Caffrey, J. L., Hsu, P. C., Chang, M. H., Faramawi, M. F. and Lin, J. W. (2012). Environmental Exposure to Dioxin-Like Compounds and the Mortality Risk in the Us Population. Int. J. Hyg. Environ. Health. 215:541-546.
Lohmann, R., Harner, T., Thomas, G. O. and Jones, K. C. (2000). A Comparative Study of the Gas-Particle Partitioning of PCDD/Fs, Pcbs, and Pahs. Environ. Sci. Technol. 34:4943-4951.
Lohmann, R. and Jones, K. C. (1998). Dioxins and Furans in Air and Deposition: A Review of Levels, Behaviour and Processes. Sci. Total Environ. 219:53-81.
McKay, G. (2002). Dioxin Characterisation, Formation and Minimisation During Municipal Solid Waste (MSW) Incineration: Review. Chem. Eng. J. 86:343-368.
Registry, A. f. T. S. a. D. (1998). Toxicological Profile for Chlorinated Dibenzo-P-Dioxins.
Schuhmacher, M. and Domingo, J. L. (2006). Long-Term Study of Environmental Levels of Dioxins and Furans in the Vicinity of a Municipal Solid Waste Incinerator. Environment International 32:397-404.
Sheu, H. L., Lee, W. J., Su, C. C., Chao, H. R. and Fan, Y. C. (1996). Dry Deposition of Polycyclic Aromatic Hydrocarbons in Ambient Air. J. Environ. Eng.-ASCE 122:1101-1109.
Shih, M., Lee, W.-S., Chang-Chien, G.-P., Wang, L.-C., Hung, C.-Y. and Lin, K.-C. (2006). Dry Deposition of Polychlorinated Dibenzo-P-Dioxins and Dibenzofurans (PCDD/Fs) in Ambient Air. Chemosphere 62:411-416.
Smith, A. G. and Gangolli, S. D. (2002). Organochlorine Chemicals in Seafood: Occurrence and Health Concerns. Food Chem. Toxicol. 40:767-779.
Suzuki, G., Nakano, M. and Nakano, S. (2005). Distribution of Pcdds/Pcdfs and Co-Pcbs in Human Maternal Blood, Cord Blood, Placenta, Milk, and Adipose Tissue: Dioxins Showing High Toxic Equivalency Factor Accumulate in the Placenta. Biosci. Biotechnol. Biochem. 69:1836-1847.
Tian, H. Z., Gao, J. J., Lu, L., Zhao, D., Cheng, K. and Qiu, P. P. (2012). Temporal Trends and Spatial Variation Characteristics of Hazardous Air Pollutant Emission Inventory from Municipal Solid Waste Incineration in China. Environ. Sci. Technol. 46:10364-10371.
Tuan, Y. J., Wang, H. P. and Chang, J. E. (2012). Formation of PCDD/Fs in the Cooling Down Process of Incineration Flue Gas. Aerosol Air Qual. Res. 12:1309-1314.
Van den Berg, M., Birnbaum, L., Bosveld, A. T. C., Brunstrom, B., Cook, P., Feeley, M., Giesy, J. P., Hanberg, A., Hasegawa, R., Kennedy, S. W., Kubiak, T., Larsen, J. C., van Leeuwen, F. X. R., Liem, A. K. D., Nolt, C., Peterson, R. E., Poellinger, L., Safe, S., Schrenk, D., Tillitt, D., Tysklind, M., Younes, M., Waern, F. and Zacharewski, T. (1998). Toxic Equivalency Factors (Tefs) for Pcbs, Pcdds, Pcdfs for Humans and Wildlife. Environ. Health Perspect. 106:775-792.
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. (2006). The 2005 World Health Organization Reevaluation of Human and Mammalian Toxic Equivalency Factors for Dioxins and Dioxin-Like Compounds. Toxicol. Sci. 93:223-241.
Wang, D. L. and Li, Q. X. (2010). Application of Mass Spectrometry in the Analysis of Polybrominated Diphenyl Ethers. Mass Spectrom. Rev. 29:737-775.
Wang, L. C. and Chang-Chien, G. P. (2007). Characterizing the Emissions of Polybrominated Dibenzo-P-Dioxins and Dibenzofurans from Municipal and Industrial Waste Incinerators. Environ. Sci. Technol. 41:1159-1165.
Wu, Y.-L., Lin, L.-F., Hsieh, L.-T., Wang, L.-C. and Chang-Chien, G.-P. (2009). Atmospheric Dry Deposition of Polychlorinated Dibenzo-P-Dioxins and Dibenzofurans in the Vicinity of Municipal Solid Waste Incinerators. Journal of Hazardous Materials 162:521-529.
校內:2018-08-27公開