底泥有機質之含量與特殊組成對多溴二苯醚吸持行為之影響

以作者查詢圖書館館藏

、以作者查詢臺灣博碩士

、以作者查詢全國書目

、勘誤回報

、線上人數：21

、訪客IP：18.191.144.47

姓名

吳雅華(Ya-Hua Wu) 查詢紙本館藏

畢業系所

環境工程研究所

論文名稱

底泥有機質之含量與特殊組成對多溴二苯醚吸持行為之影響
(The influence of sediment organic matter content and distinctive composition on the sorption of polybrominated diphenyl ethers)

相關論文

★ 工業廢水對灌溉水質影響之研究-以黃墘溪為例	★ 廢冷陰極管汞回收處理效率之研究
★ 室內懸浮微粒與生物氣膠之相關性探討-以某醫學中心為例	★ 化學機械研磨廢液對工業區污水處理效益與操作成本之影響
★ 網路數位電力監測系統於大學用電行為分析之研究	★ 光電業進行自願性碳標準(VCS)減量計畫可行性之研究
★ 污染農地整治後未能符合農用成因之探討	★ 桃園縣居家入侵紅火蟻防治方法探討
★ 印刷電路板產業濕式製程廢液回收鈀金屬可行性之研究	★ 不同表面特性黏土催化高分子凝聚劑與消毒劑(氯)反應之研究
★ 界面活性劑對土壤/水系統中有機污染物分佈行為之研究	★ 淨水程序中添加高分子凝聚劑對混凝與加氯處理效應之研究
★ 土壤無機相對揮發性有機污染物吸∕脫附行為之影響	★ 土壤對Triton 系列各EO鏈選擇性吸附之研究
★ 土壤有機質對土壤/水系統中低濃度非離子有機污染物吸附行為之研究	★ 不同表面特性黏土催化水中有機物之氯化反應研究

檔案

[Endnote RIS 格式]

[Bibtex 格式]

[相關文章]

[文章引用]

[完整記錄]

[館藏目錄]

[檢視]

[下載]

本電子論文使用權限為同意立即開放。
已達開放權限電子全文僅授權使用者為學術研究之目的，進行個人非營利性質之檢索、閱讀、列印。
請遵守中華民國著作權法之相關規定，切勿任意重製、散佈、改作、轉貼、播送，以免觸法。

摘要(中)

多溴二苯醚因結構穩定、水中溶解度低、不易被破壞且和小顆粒的粒子及煤灰有很強的結合力，故有積蓄在底泥中的傾向，經由檢測研究標的底泥多溴二苯醚含量結果，不論河川水庫底泥皆發現有多溴二苯醚之存在，且濃度均以高溴數之多溴二苯醚為主，顯示高溴數的多溴二苯醚比低溴數更易累積在環境中。
為釐清影響多溴二苯醚於水環境中傳輸與宿命的因子，因此利用河川、水庫中具不同有機質特性之底泥進行吸附實驗。實驗結果顯示，河川水庫底泥對多溴二苯醚的吸附等溫線皆呈線性，顯示自然水體中多溴二苯醚以分佈作用吸持至底泥之有機質中。多溴二苯醚之分佈常數K值主要受底泥的來源及有機質含量所影響，而底泥比表面積、平均孔洞直徑對多溴二苯醚之分佈常數K值影響不大。對同一種多溴二苯醚而言，不論河川或水庫中底泥所得之log Kom值大致相同。當底泥有機質含量相同時，log Kom值會受脂肪族碳含量多寡的影響。含不同溴數之多溴二苯醚，其log Kom值隨溴原子數目之增加而上升；含相同溴數、不同苯環位置之多溴二苯醚，其logKom值受化合物之水溶解度及溴原子位置所影響。

摘要(英)

Polybrominated diphenyl ethers (PBDEs) have shown strong binding abilities to small particles, such as dust, due to their structure stabilities and low water solubilities. As a result, these compounds tend to accumulate in sediments. When sediments collected from different reservoirs and rivers are subjected to the analysis, the results obtained detected the existence of PBDEs. It is clear from these data that compounds with higher bromine numbers are much more easily been accumulated in the environment than compounds with lower bromine numbers.
The main purpose of this study was focused on the major factors that affect the transportation and fate of polybrominated diphenyl ethers in natural water. The adsorption experiment of polybrominated diphenyl ethers was examined by collecting the organic matter under different characteristics of the sediments. The results of this experimental show the adsorption isotherms of PBDEs by sediment is proportional to the distribution and composition of organic matter contents. The partition coefficient K value of PBDEs is strongly affected by the organic matter content of the sediment. The specific surface area, average pore diameter of the sediment do not effect significantly the partition coefficient K value of PBDEs. On the same of PBDEs, regardless of whether the river and reservoir sediments, normalized partition coefficient (Kom) value is similar. When organic matter content of the sediment is same, the log Kom values affected by the amount of aliphatic carbon content. If, the number of bromine atoms of different PBDEs is different, the log Kom value increase as the number of bromine atoms increases.

關鍵字(中)

★ log Kom
★ 有機質含量
★ 多溴二苯醚
★ 吸持行為

關鍵字(英)

★ Organic matter contant
★ Sorption
★ Polybrominated diphenyl ethers
★ log Kom

論文目次

目錄…………………………………………………………………I
圖目錄………………………………………………………………V
表目錄………………………………………………………………VIII
第一章前言…………………………………………………………1
1-1 研究緣起……………………………………1
1-2 研究目的與內容……………………………3
第二章文獻回顧…………………………………………………4
2-1 溴化阻燃劑之種類與應用………………4
2-2 多溴二苯醚之介紹………………………6
2-2-1 多溴二苯醚之基本特性……8
2-2-2 多溴二苯醚於環境中之流佈…10
2-2-3 多溴二苯醚的毒理作用………14
2-2-4 多溴二苯醚目前管制策略……16
2-3 土壤基本特性……………………………17
2-3-1 土壤無機質…………………17
2-3-2 土壤有機質…………………18
2-4 土壤對有機污染物之吸持作用………19
2-4-1 吸附理論…………………19
2-4-2 分佈理論…………………20
2-4-3 土壤於含水環境下之吸持作用…21
2-5 底泥有機質對有機污染物吸持行為之影響…………………………... 23
第三章實驗材料與方法…………………………………………………………….. 27
3-1 實驗內容................................................................................................... 27
3-2 PBDEs分析方法之建立.......................................................................... 29
3-2-1 環境背景PBDEs之檢測方法...................................................... 29
3-2-2 底泥吸持實驗PBDEs之檢測方法............................................. 34
3-3 底泥相關結構分析................................................................................... 35
3-4 環境背景分析........................................................................................... 43
3-4-1 實驗室灰塵PBDEs濃度分析...................................................... 43
3-4-2 底泥樣品PBDEs濃度分析.......................................................... 44
3-5 水庫和河川底泥PBDEs之吸持實驗……………………………......... 47
3-5-1 PBDEs於底泥-水系統中有機質分佈常數(Kom)之計算............ 51
3-6 實驗藥品................................................................................................... 53
3-6-1 PBDEs標準品.............................................................................. 53
3-6-2 其他實驗藥品............................................................................... 53
3-7 實驗設備................................................................................................... 55
第四章結果與討論…………………………………………………………………... 57
4-1 分析條件的建立與底泥理化特性分析………………………............... 57
4-1-1 PBDEs之HRGC/HRMS分析條件的建立……………………. 57
4-1-2 研究標的底泥之理化特性分析……………………………...... 63
4-1-3 吸附實驗之檢量線…..………………………………………… 70
4-2 環境背景分析結果…..……………..……………..…………………… 74
4-2-1 實驗室灰塵PBDEs之濃度…..……………..…………………. 74
4-2-2 水庫及河川底泥樣品中PBDEs 濃度…..……………………. 76
4-2-3 底泥中有機質含量與PBDEs含量之關係…..………………... 81
4-3 PBDEs於土壤/水飽和系統中之吸持作用.. …..……………………… 82
4-3-1 PBDEs於水庫底泥之吸持作用…..…………………………… 83
4-3-2 PBDEs於河川底泥之吸持作用…..…………………………… 87
4-4 PBDEs分佈常數之影響因子…..……………..……………………….. 92
4-4-1 不同來源底泥對PBDEs分佈常數之影響…..………………... 92
4-4-2 底泥比表面積對PBDEs分佈常數之影響…..……………….. 96
4-4-3 底泥有機質含量對PBDEs分佈常數之影響…..…………….. 98
4-4-4 底泥質地對PBDEs分佈常數之影響…..……………………... 101
4-4-5 底泥pH值對PBDEs分佈常數之影響…..……………………. 104
4-5 不同有機質組成對PBDEs校正常數Kom之影響…..…………………. 106
4-5-1 底泥有機質官能基對PBDEs Kom之影響….............................. 109
4-5-2 不同來源底泥對PBDEs Kom之影響…...................................... 113
4-5-3 翡翠水庫上中下游底泥對PBDEs Kom之影響……………….. 115
4-5-4 河川底泥對PBDEs Kom之影響….............................................. 117
4-6 不同PBDEs同源物對底泥分佈常數之影響…...................................... 119
4-6-1 不同溴數PBDEs之log Kom變化…........................................... 119
4-6-2 相同溴數PBDEs之log Kom變化…............................................ 121
4-7 PBDEs之估算與實驗Kom值…..………...…..………...…..………..... 126
第五章結論……….………………………………………………………………...... 128
5-1 結論……………………………………………………………………... 128
5-2 建議……………………………………………………………………... 130
第六章參考文獻……………………………………………………………………... 131

參考文獻

? Allchin, C. R.., Law, R. J., Morris, S., “Polybrominated diphenyl ethers in sediment and biota downstream of potential sources in the UK”, Environmental Pollution, 105, 197-207, 1999.
? Alocok, R. E., Sweetman, A., Jones, K. C., “Assessment of organic contaminant fate in waste water treatment plants. I: Selected compounds and physicochemical properties”, Chemosphere, 10, 2247-2262, 1999.
? Bieniek, D. M., Bahadir, F. K., “Formation of heterocyclic hazardous compounds by thermal degradation of organic compounds”, Heterocyles, 28, 719-722, 1989.
? Booij, K., Zegers, B. N., Boon, J. P., “Levels of some polybrominated diphenyl ether (PBDE) flame retardants along the Dutch coast as derived frpm their accumulation in SPMDs and blue mussels (Mytilus edulis) ”, Organohalogen Compounds, 47, 89-92, 2000.
? Brady, N. C., “ The nature and properties of soils”, Macmillan, New York, USA, 693, 1974.
? Braek velt, E., Tittlemier, S. A., Tomy, G. T., “Diret measurement of octanol-water partition coefficients of some environmentally relevant brominated diphenyl ether congeners”, Chemosphere, 51, 563-567, 2003.
? Bromine Science and Environmental Forum. http://www.bsef.com/，2006.
? BSEF. Major Brominated Flame Retardants Volume Estimates: Total Market Demand By Region in 2001. Brussels: Bromine Science and Environmental Forum.
? Chen, B., Johnson, J., Chefetz, B., Zhu, L., Xing, B., “Sorption of polar and nonploar aromatic organic contaminants by plant cuticular materials:Role of polarity and accessibility”, Environmental Science and Technology, 39, 6138-6146, 2005.
? Chernyak, S. M., Batterman, S. A., Godwin, C. C., Jia, C., Charles, S. M., “Evolution of flame retardant chemicals in a newly constructed building”, Organohalogen Compounds, 69, 994-997, 2007.
? Chiou, C. T., Jiunn, F. L., Stephen, A. B., “The Surface Area of Soil Organic Matter”, Environmental Science and Technology, 24, 1164-1166, 1990.
? Chiou, C. T., Shoup, T. D.,“Soil sorption of organic vapors and effect of humidity on sorptive mechanism and capacity”, Environmental Science and Technology, 19, 1196-1200, 1985.
? Chiou, C. T., Louis, J. P., Virgil, H. F., “A Physical Concept of Soil-Water Equilibria for Nonionic Organic Compounds”, Science, 206, 831-832, 1979.
? Chiou, C. T., Porter, P. E., Schmedding, D. W., “Partition equilibria of nonionic organic compounds between soil organic matter and water”, Environmental Science and Technology, 17, 227-231, 1983.
? Covaci, A., de Boer, J., Ryan, J. J., Voorspoels, S., Schepens, P., “Determination of polybrominated diphenyl ethers and polychlorinated biphenyls in human adipose tissue by large-volume injection-narrow-bore capillary gas chromatography/electron impact low-resolution mass spectrometry”, Analysis Chemical, 74, 790-798, 2002a.
? Darnerud, P. O., Eriksen, G. S., Johannesson, T., “Polybrominated Diphenyl Ethers: Occurrence, Dietary Exposure, and Toxicology”, Environmental Health Perspectives , Reviews in Environmental Health, 109, 49-68, 2001.
? Darnerud, P. O., “Toxic effects of brominated flame retardants in man and in wildlife”, Environment International, 29, 841-853, 2003.
? de Wit, C. A., “An overview of brominated flame retardants in the environment”, Chemosphere, 46, 583-24, 2002.
? Dodder, N., Strandberg, B., Hites, R. A., “Concentrations and spatial variations of polybrominated diphenyl ethers in fish and air from the North-Eastern United States”, Environmental Science and Technology, 36, 146-151, 2002.
? Goring, C. A. I., “Control of nitrification by 2-chloro-6-(trichloro-methyl) pyridine, Soil Science, 93, 211-218, 1962.
? Grathwohl, P., “Influence of organic matter from soils and sediments from various organicon the sorption of some chlorinated aliphatic hydrocarbons : implications on Koc correlations”, Environmental Science and Technology, 24, 1687-1693, 1990.
? Hardy, M. L., “The toxicology of the three commercial polybrominated diphenyl oxide (ether) flame retardants”, Chemosphere, 46, 757-777, 2002.
? Hassanin, A., Breivik, K., Meijer, S. N., Steinnes, E., Thomas, G. O., Jones, K. C., “PBDEs in European background soils: levels and factors controlling their distribution”, Environmental Science and Technology, 38, 738-745, 2004.
? Hatcher, P. G., Schnitzer, M., Dennis, L.W., Maciel, G. E., “Aromaticity of humic substances in soils”. Soil Science Society of America Journal, 45, 1089-1094, 1981.
? Hooper, K., McDonald, T. A., “The PBDEs: an emerging environmental challenge and another reason for breast milk monitoring programs”, Environmental Health. Perspect, 108, 387-392, 2000.
? Ikonomou, M., Rayne, S., Fischer, M., Fernandez, M., Cretney, W., “Occurrence and congener profiles of polybrominated diphenyl ethers (PBDEs) in environmental samples from coastal British Columbia”, Canada, Chemosphere, 46,649– 63, 2002a.
? Jenny, H., “Factor of soil formation”, McGraw-Hill, New York, 1941.
? Kile, D. E., Chiou, C. T., Zhou, H., Li, H., Xu, O., “Partition of Nonpolar Organic Pollutants from Water to Soil and Sediment Organic Matters”, Environmental Science and Technology, 29, 1401, 1995.
? Kono, Y., Fukuzawa, E., Miyazaki, M., Nomura, T., Komatsu, K., “Polybrominated dioxins (PBDDs/DFs) and polybrominated diphenyl ethers (PBDEs) in house dust in ordinary homes”, Organohalogen Compounds, 69, 2781-2784, 2007.
? Kononova, M. M., “Soil organic matter, Pergamon”, New York, USA, 450, 1961.
? Lambert, S. M., J. Agric, “Functional Relationship Between Sorption in Soil and Chemical Structure”, Food Chemicals, 15, 572-576, 1989.
? Lambert, S. M., Porter, P. E., Schieferstein, R. H., “Movement and sorption of chemicals applied to the soil.” Weed, 13, 185-190, 1965.
? McDonald, T. A., “A perspective on the potential health risks of PBDEs”, Chemosphere, 46, 745-755, 2002.
? Onken, B. M., S. J. Traina, “The sorption of pyrene and anthracene to humic acid-mineral complexes: effect of fractional organic carbon content”, Journal of Environmental Quality, 26, 126-132, 1997.
? Pijnenburg, A. M., Evert, J. W., Boer, J. de., Boon, J. P., “Polybrominated biphenyl and biphenyl ether flame retardants: analysis toxicity and environmental occurrence”, Reviews of Environmental Contamination and Toxicology, 141, 1-26, 1995.
? Rutherford, D. W., Chiou, C. T., “Effect of Water Saturation in Soil Organic Matter on the Partition of Organic Compounds,” Environmental Science and Technology, 26, 965- 970, 1992.
? Salloum, M.J., Dudas, M. J., McGill, W. B., “Variation of 1-naphthol sorption with organic matter fractionation: the role of physical conformation”, Organic Geochemical, 32, 709-719, 2001.
? Kang, S., Xing, B., “Phenanthrene sorption to sequentially extracted soil humic acids and humans”, Environmental Science and Technology, 39, 134-140, 2005.
? Sjӧdin, A., HãKan, C., Kaj, T., Sverker, S., Ãke, B., Conny, Ő.,“Flame retardants in indoor air at an electronics recycling plant and at other work environments”, Environmental Science and Technology, 35, 448-454, 2001.
? Stapleton, H., Dodder, N., Schantz, M., Wise, S., Organohalogen Compounds, 66, 3741, 2004.
? Stevenson, F. J., “Humus Chemistry”, John Wiley & Sons, Somersel, NJ, 17, 1982.
? Thomas, D. B., Ӧrjan, G., “Soot sorption of non-ortho and ortho substituted PCBs”, Chemosphere, 53, 515-522, 2003.
? Tittlemier, S.A., Halldoroson, T., Stern, G. A., Tomy, G. T., “Vapor pressures, aqueous solubilities, and Henery’s Law Constants of some brominated flame retardants”, Environmental Toxicology Chemical, 21, 1804-1810, 2002.
? Watanabe, I., Sakai, S., “Environmental release and behavior of brominated flame retardants”, Environment International, 29, 665-682, 2003.
? Watanabe, I., Tatsukawa, R., “Anthropogenic brominated aromatics in the Japanese environment. In: Proceedings: Workshop on Brominated Aromatic Flame Retardants”, Swedish National Chemicals Inspectorate, Solna, Sweden, 1990.
? WHO, Environmental Health Criteria 162. Brominated diphenyl ethers, International Program on Chemical Safety, World Health Organization, Geneva, Switzerland, 1994.
? WHO/IPCS. Chlorinated Paraffins. Environmental Health Criteria 181, 1996.
? 江政傑，“台灣西南海域沉積物中持久性有機化合物含量分佈之研究”，國立中山大學海洋環境及工程學系碩士論文，2006。
? 李俊璋、吳幸娟，“樹脂製造業勞工空氣中多溴二苯醚暴露調查研究”，勞工委員會勞工安全衛生研究所， 2007。
? 楊逸帆，“土壤有機質芳香性對非離子有機化合物分佈行為之影響”，國立中央大學環境工程研究所碩士論文，2003。
? 張怡塘，“有效遏阻火災的利器-溴化阻燃劑”，工程科技資訊，2009。
? 陳重羽，“台灣地區主要河川多溴聯苯醚污染分佈研究”，國立成功大學環境醫學研究所碩士論文，2005。
? 行政院環保署，公告毒性化學物質一覽表，1995。
? 行政院環境保護署，土壤酸鹼值（pH 值）測定方法－電極法，NIEA S410.62C，中華民國97年10月2日。
? 行政院環境保護署，多溴二苯醚檢測方法－氣相層析卅高解析質譜法 NIEA M802.00B，中華民國96年8月15日。
? 行政院環境保護署，底泥採樣方法NIEA S104.30C，中華民國92年11月24日。
? 行政院環境保護署，環境檢驗方法偵測極限測定指引NIEA PA107，中華民國94年1月15日。

指導教授

李俊福(Jiunn-Fwu Lee)

審核日期

2010-8-23

推文