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博碩士論文 etd-0901104-183506 詳細資訊
Title page for etd-0901104-183506
論文名稱
Title
腐植酸混合效應對多環芳香烴碳氫化合物與溶解性有機物結合係數之影響—動力學研究
The Study of Kinetic Effect by Mixing Binary Humic Acids on the Binding Constants of Polycyclic Aromatic Hydrocarbons and Dissolved Organic Matter
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
142
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2004-07-29
繳交日期
Date of Submission
2004-09-01
關鍵字
Keywords
螢光衰減法、腐植酸、多環芳香烴碳氫化合物、動力學、結合係數
fluorescence quenching method, kinetic, binding constant, PAHs, humic acid
統計
Statistics
本論文已被瀏覽 5657 次,被下載 1845
The thesis/dissertation has been browsed 5657 times, has been downloaded 1845 times.
中文摘要
河口地區受到海、淡水團交互的影響下,並且擁有陸源及海源不同特性的溶解性有機物混合,因此其與疏水性有機物間的吸附行為更加複雜難料。本研究以螢光衰減法來探討pyrene與兩種溶解性有機物(SHHA與LHA及SRNOM與LHA)混合時之結合係數(Kdoc),藉以釐清PAHs與不同來源特性的溶解性有機物混合時之吸附機制。
在探討pyrene和SHHA與LHA及SRNOM與LHA混合間之結合係數時,發現SHHA與LHA及SRNOM與LHA之混合動力學對其結合係數有著重大的影響,若SHHA與LHA及SRNOM與LHA混合溶液沒有足夠的靜置時間,將導致其結合係數產生偏差影響實驗結果。研究中發現DOMs間的混合作用對其與pyrene間的結合係數具有保守性作用(conservative effect)。此外從不同混合比例之初始攪拌效率中,發現SRNOM與LHA之混合機制是屬於單純的擴散效應;但SHHA與LHA混合機制並不只是受到擴散效應影響,另有可能受到其他因子的影響,有待進一步的研究。
Abstract
Estuary is a complex region due to the mixing of fresh and sea water as well as the mixing of terrestrial and marine dissolved organic matters (DOM), so that the sorption behavior between hydrophobic organic compounds and dissolved organic matters is very complicated to estimate. By applying fluorescence quenching method, we investigated the influence of the mixing of binary dissolved organic matters from different sources on the binding constant (Kdoc) of pyrene and DOM.

Results show that the kinetic of mixing of binary DOMs influences the binding constant, that means if there weren’t enough standing time for mixing of binary DOMs, it would cause some bias in estimating the binding constants of pyrene and DOMs mixture. In this study, we also found that there exists a linear relationship on the binding constants between pyrene and DOMs mixture against mixing ratios. In addition, the mixing mechanism of SRNOM and LHA was dominated by diffusion process from the results of initial mixing efficiency. However, the diffusion process might not be the only mechanism of the mixing reaction of SHHA and LHA, other factors should be considered. Further investigations should be done to find out the dominating factors on the mixing of SHHA and LHA system in the future.
目次 Table of Contents
第一章 前言 1
第二章 文獻回顧 3
2-1 疏水性有機污染物 3
2-1-1 何謂疏水性有機污染物? 3
2-1-2 多環芳香烴碳氫化合物 3
2-2 溶解性有機物 7
2-2-1 何謂溶解性有機物? 7
2-2-2 腐植質概述 8
2-3 DOM來源特性與PAHs結合力之關聯 12
第三章 實驗材料及方法 14
3-1 實驗材料 14
3-2 實驗方法 15
3-2-1 實驗方法的選用 15
3-2-1 螢光衰減法原理概述 18
3-3 校正公式 21
3-4 實驗步驟 22
第四章 結果與討論 25
4-1 螢光衰減理論應用之確立 25
4-2 兩種相異特性DOMs共存競爭效應 27
4-3 動力學實驗 30
4-3-1 SHHA與LHA共存之混合動力學 30
4-3-2 SRNOM與LHA共存之混合動力學 47
4-4 SHHA(LHA)與SRNOM(LHA)混合競爭效應 61
4-5 SHHA(LHA)與SRNOM(LHA)之初始攪拌增加效率比較 64
第五章 結論與建議 65
5-1 結論 65
5-2 建議 67
參考文獻 68
附 錄 73
參考文獻 References
Chen, S., Inskeep, W. P., Williams, S. A. and Callis, P. R. (1992) Complexation of 1-naphthol by humic and fulvic acids. Soil Sci. Soc. Am. J. 56, 67-73.

Chen, S., Inskeep, W. P., Williams, S. A. and Callis, P. R. (1994) Fluorescence lifetime measurements of fluoranthere, 1-naphthol, and Napropamide in the presence of dissolved humic acid. Environ. Sci. Technol. 28, 1582-1588.

Chin, Y-P, Aiken, G. R. and O’Loughlin, E. (1994) Molecular weight, polydispersity, and spectroscopic properties of aquatic humic substances. Environ. Sci. Technol. 28, 1853-1858.

Chin, Y-P, Aiken, G. R. and Danielsen, K. M. (1997) Binding of pyrene to aquatic and commercial humic substances: the role of molecular weight and aromaticity. Environ. Sci. Technol. 31, 1630-1635.

Chiou, C. T., Schmedding, D. W. and Manes, M. (1982) Partitioning of organic compounds in octanol-water systems. Environ. Sci. Technol. 16, 4-10.

Chiou, C. T. (1985) Partition coefficients of organic compounds in lipid-water systems and correlations with fish bioconcentration factors. Environ. Sci. Technol. 19, 57-62.

Chiou, C. T., Shoup, T. D. and Poter, P. E. (1985) Mechanistic roles of soil humus and minerals in the sorption of nonionic organic compounds from aqueous and organic solutions. Org. Geochem. 8, 9-14.


Chiou, C. T., Malcolm, R. L., Birnton, T. I. and Kile, D. E. (1986) Water solubility enhancement of some organic pollutants and pesticides by dissolved humic and fulvic acids. Environ. Sci. Technol. 20, 502-508.

Danielsen, K. M., Chin, Y-P, Buterbaugh, J. S., Gustafson, T. L. and Traina, S. J. (1995) Solubility enhancement and fluorescence quenching of pyrene by humic substances: The effect of dissolved oxygen on quenching processes. Environ. Sci. Technol. 29, 2162-2165.

Futoma, D. J., Smith, S. R., Smith, T. E. and Tanaka, J. (1981) The analysis of polycyclic aromatic hydrocarbons in water system, CRC Press, Florida.

Gauthier, T. D., Shane, E. C., Guerin, W. F., Seitz, W. R. and Grant, C. L. (1986) Fluorescence quenching method for determining equilibrium constants for polycyclic aromatic hdyrocarbons binding to dissolved humic matterials. Environ. Sci. Technol. 20, 1162-1166.

Herbert, B. E., Bertsch, P. M. and Novak, J. M. (1993) Pyrene sorption by water-soluble organic carbon. Environ. Sci. Technol. 27, 398-403.

Johnson, W. P. and Amy, G. L. (1995) Facilitated transport and enhanced desorption of polycyclic aromatic hydrocarbons by natural organic matter in aquifer sediments. Environ. Sci. Technol. 29, 807-817.

Lakowicz, J. R.(1983) Principles of fluorescence spectroscopy, Plenum Press, New York.


Landrum, P. F. Nihart, S. R., Eadie, B. J. and Gardner, W. S. (1984) Reverse-phase separation method for determining pollutant binding to aidrich humic acid and dissolved organic carbon of natural water. Environ. Sci. Technol. 18, 187-192.

Lee, C-L, Huang, H-T, Kuo, L-J and Hsieh, P-C (2003) Effects of ionic strength on the binding of phenanthrene and pyrene to humic substances: three-stage variation model. Wat. Res. 37, 4250-4258.

Magee, B. R., Lion, L. W. and Lemly, A. T. (1991) Transport of dissolved organic macromolecules and their effect on the transport of Phenanthrene in porous media. Environ. Sci. Technol. 25, 323-331.

McCarthy, J. F. and Jimenez, B. D. (1985) Interactions between polycyclic aromatic hydrocarbons and dissolved humic material: binding and dissociation. Environ. Sci. Technol. 19, 1072-1076.

Miller, M. M., Wasik, S. P., Huang, G-L, Shiu, W-Y and Mackay, D. (1985) Ralationships between octanol-water partition coefficient and aqueous solubility. Environ. Sci. Technol. 9, 522-529.

Morra, M. J., Corapcioglu, M. O., Wandruszka, R. V., Marshall, D. B. and Topper, K. (1990) Fluorescence quenching and polarization studies of Naphthalene and 1-Naphthol interaction with humic acid. Soil Sci. Soc. Am. J. 54, 1283-1289.

Paolis, F. D. and Kukkonen, J. (1997) Binding of organic pollutants of humic and fulvic acids : Influence of pH and the structure of humic material. Chemosphere. 34, 1693-1704.

Parker, C. A. (1968) Photoluminescence of solutions. Elsevier Amsterdam.
Ragle, C. S., Engebretson R. R. and Wandruszka, R. V. (1997) The sequestration of hydrophobic micropollutants by dissolved humic acids. Soil Sci. 62, 106-114.

Rav-acha, Ch. and Rebhun, M. (1992) Binding of organic solutes to dissolved humic substances and its effects on adsorption and transport in the aquatic environment. Wat. Res. 26, 1645-1654.

Rebhun, M., Smedt, F. DE and Rwetabula, J. (1996) Dissolved humic substances for remediation of sites contaminated by organic pollutants: Binding-desorption model prdicitions. Wat. Res. 30, 2027-2038.

Rutherford, D. W., Chiou, C. T. and Kile, D. E. (1992) Influence of soil organic matter composition on the partition of organic compounds. Environ. Sci. Technol. 26, 336-340.

Schlautman, M. A. and Morgan, J. J. (1993) Effects of aqueous chemistry on the binding of polycyclic aromatic hydrocarbons by dissolved humic materials. Environ. Sci. Technol. 27, 961-969.

Shimziu, Y. and Liljestrand, H. M. (1991) Sorption of polycyclic aromatic hydrocarbons onto natural solids: Determination by fluorescence quenching method. Wat. Sci. Technol. 23, 427-436.

Stevenson, F. J. (1994) Humus Chemistry: genesis, composition, reactions, 2nded., John Wiley & Sons, New York.

Tiller, C. L. and Jones, K. D. (1997) Effect of dissolved oxygen and light exposure on determination of Koc values for PAHs using fluorescence quenching. Environ. Sci. Technol. 31, 424-429.

Traina, S. J., Spontak, D. A. and Logan, T. J. (1989) Effect of cations on complexation of Naphthalene by water-soluble organic carbon. Environ. Qual. 18, 221-227.



Voice, T. C., Rice, C. P. and Weber, W. J., Jr. (1983) Effect of solids concentration on the sorptive partitioning of hydrophobic pollutants in aquatic systems. Environ. Sci. Technol. 17,513-518.

Wershaw, R. L. (1986) A new model for humic materials and their interactions with hydrophobic organic chemicals in soil-water or sediment-water systems. J. Contamin. Hydro. 1, 29-45.

Wershaw, R. L. (1989) Application of a membrane model to the sorptive interactions of humic substances. Environ. Health Perspectives 83, 191-203.

Wershaw, R. L. (1993) Model for humics in soils and sediments. Environ. Sci. Technol. 27, 814-816.

Zhou, J. L., Rowland, S. and Mantoura, R. F. C. (1994) The formation of humic coatings om mineral particles under simulated estuarine conditions – a mechanistic study. Wat. Res. 28, 571-579.

Zhou, J. L., Rowland, S. and Mantoura, R. F. C. (1995b) Partition of synthetic pyrethroid insecticides between dissolved and particulate phases. Wat. Res. 29, 1023-1031.

Zhou, J. L. and Rowland, S. J. (1997) Evaluation of the interactions between hydrophobic organic pollutants and suspended particles in estuarine waters. Wat. Res. 31, 1708-1718.

陳鎮東 (1994),海洋化學,國立編譯館,台北市。
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