多溴聯苯醚 (polybrominated diphenyl ether，PBDEs)為溴化阻燃劑的一種，近30年來已被廣泛地運用，但目前仍少有研究探討其對水生底棲生物之毒性影響。單孔蚓是台灣的常見水生寡毛類，且為重要餌料生物，故本研究探討PBDEs對單孔蚓的存活率與蛋白質表現之影響。將單孔蚓曝露於BDE-47 (tetra-BDE)與BDE-183 (hepta-BDE)中，以單孔蚓之體重變化、產卵繭數、存活率及蛋白質表現來評估BDE-47與BDE-183之毒性。結果顯示，經兩週處理後， BDE-47各濃度皆不影響單孔蚓體重、生殖與存活率；曝露八週後，僅700 ng/g BDE-47與BDE-183組之產卵繭數減少且存活率顯著降低(p<0.05)，其存活率分別為48±14與3±3％，1-100 ng/g BDE-47與BDE-183對存活率則無顯著影響，BDE-47與BDE-183之LC50、LT50分別為2311與169 ng/g、47與19天；由蛋白質二維電泳之叢集分析結果得知100 ng/g BDE-47對40個蛋白質表現的影響與10 ng/g BDE-183相似，表示低濃度BDE-183即與100 ng/g BDE-47有著相似的影響力，皆顯示BDE-183的毒性可能較BDE-47強；而低濃度如1 ng/g BDE-47與BDE-183處理八週不影響單孔蚓之存活率，卻顯著影響其蛋白質表現強度，表示由蛋白質階層來檢視污染物的毒性具較高的敏感度。

The current knowledge concerning effects of polybrominated diphenyl ether (PBDEs) on benthic aquatic organisms is still very limited although they have been widely used as fire retardant additives for 3 decades. This study was conducted to evaluate the toxic effects of BDE-47 and BDE-183, the two common congeners of PBDEs in river sediments, on a benthic oligochaete worms, Monopylephorus limosus. The worms were exposed to BDE-47 or to BDE-183 for two or eight weeks. The survival rates of M. limosus decreased significantly when exposed to 700 ng/g dry soil of BDE-47 or BDE-183 for 8 weeks, but not in groups of 1-1000 ng/g BDE-47 for 2 weeks. A total of forty proteins of M. limosus has been expressed and determined by the two-dimensional gel electrophoresis (2-DE). Through the cluster analysis, it was found that the protein expression in the group of 100 ng/g BDE-47 was similar to 10 ng/g BDE-183. The results indicate that the toxicity of BDE-183 was greater than BDE-47 to M.limosus. Although the survival rate of M. limosus was not significantly affected when exposed to BDE-47 or BDE-183 at concentrations of 1 to 100 ng/g, significant differences in protein expression were found. Thus, the analysis of protein expression is more sensitive to detect the toxicological change in M. limosus than the survival test.

謝辭……………………………………………………… i
中文摘要………………………………………………… ii
英文摘要………………………………………………… iii
目錄……………………………………………………… iv
表目錄…………………………………………………… v
圖目錄…………………………………………………… vi
附錄目錄………………………………………………… vii
第一章 多溴聯苯醚之文獻回顧…………………………1
第二章 前言………………………………………………13
第三章 材料與方法………………………………………17
第四章 結果………………………………………………24
第五章 討論………………………………………………30
參考文獻………………………………………………… 37
附表……………………………………………………… 46
附圖……………………………………………………… 49
附錄……………………………………………………… 65
個人履歷………………………………………………… 87

Alaee, M., J. Luross, D. B. Sergeant, D.C.G. Muir, D. M. Whittle, and K. Solomon. 1999. Distribution of polybrominated diphenyl ethers in the Canadian environment. Organohalogen Compounds 40:347-350.
Alaee, M., and R. Wenning. 2002. The significance of brominated flame retardants in the environment: current understanding, issues and challenges. Chemosphere 46:579-582.
Allchin, C. R., R. J. Law, and S. Morris. 1999. Polybrominated diphenylethers in sedments and biota downstream of potential sources in the UK. Environmental Pollution 105:197-207.
Back, H. 1990. Epidermal uptake of Pb, Cd, and Zn in tubificid worms. Oecologia 85:226-232.
Bergander, L., A. Kierkegarrd, U. Sellstrome, U. Wideqvist, and C. de Wit. 1995. Are brominated flame retardants present in ambient air? 6th Nordic Symposium on Organic Pollutants, Smygehuk.
Bhat, M. K., C. l. Yu, N. Yap, Q. Zhan, Y. Hayashi,, and a. S. y. C. P. Seth. 1997. Tumor suppressor p53 is a negative regulator in thyroid hormone receptor signaling pathways. The journal of biological chenistry 272:28989-28993.
Bocio, A., J. M. Llobet, J. L. Domingo, J. Corbella, A. Teixidoa, and C. Casass. 2003. Polybrominated diphenyl ethers (PBDEs) in foodstuffs: human exposure through the diet. Journal of Agricultural and Food Chemistry 51: 3191-3195.
Bosworth, C. A., C. W. Chou, R. B. Cole, and B. B. Rees. 2005. Protein expression patterns in zebrafish skeletal muscle: initial characterization and the effects of hypoxic exposure. Proteomics 5:1362-1371.
Bouche, M. L., F. Habets, S. Biagianti-Risbourg, and G. Vernet. 2000. Toxic effects and bioaccumulation of cadmium in the aquatic oligochaete Tubifex tubifex. Ecotoxicology and Environmental Safety 46:246-251.
Branchi, I., E. Alleva, and L. G. Costa. 2002. Effects of perinatal exposure to a polybrominated diphenyl ether (PBDE 99) on mouse neurobehavioural development. NeuroToxicology 23:375-384.
Breitholtz, M., and L. Wollenberger. 2003. Effects of three PBDEs on development, reproduction and population growth rate of the harpacticoid copepod Nitocra spinipes. Aquatic Toxicology 64:85-96.
Burreau, S., J. Axelman, D. Broman, and E. Jacobsson. 1997. Dietary uptake in pike (Esox lucius) of some polychlorinated biphenyls, polychlorinated naphthalenes and poly brominated diphenyl ethers administered in a natural diet. Environmental Toxicology and Chemistry 16:2508-2513.
Burreaua, S., D. Broman, and U. Orn. 2000. Tissue distribution of 2, 2', 4, 4'-tetrabromo[14C]diphenyl ether ([14C]-PBDE 47) in pike (Esox lucius) after dietary exposure - a time series study using whole body autoradiography. Chemosphere 40:977-985.
Cheng, I. J. 1995. The temporal changes in benthic abundances and sediment nutrients in a mudflat of the Chuwei Mangrove Forest, Taiwan. Hydrobiologia 295:221-230.
Christensen, J. H., M. Glasius, M. Pecseli, J. Platz, and G. Pritzl. 2002. Polybrominated diphenyl ethers (PBDEs) in marine fish and blue mussels from southern Greenland. Chemosphere 47:631-638.
Christer, E., and P. Andreina. 1986. An Italian record of the aquatic oligochaeta Monopylephorus limosus (Tubificidae), previously known only from Japan and China. Bollettino di Zoologia 53:115-118.
Christer, E., and H. L. Hsieh. 1997. Records of estuarine Tubificidae (Oligochaeta) from Taiwan. Species Diversity 2:97-104.
Covaci, A., J. de Boer, J. J. Ryan, S. Voorspoels, and P. Schepens. 2002. 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. Analytical Chemistry 74:790-798.
Darnerud, P. O., and A. Thuvander. 1998. Studies on immunological effects of polybrominated diphenyl ethers (PBDE) and polychlorinated biphenyls (PCB) exposure in rats and mice. Organohalogen Compounds 35:415–418.
De Boer, J. 1990. Brominated diphenyl ethers in Dutch freshwater and marine fish. Organohalogen Compounds 2:315-318.
De Boer, J., P. G. Wester, H. J. G. Klamer, W. E. Lewis, and J. P. Boon. 1998. Do flame retardants threaten ocean life? Nature 394:28-29.
De Boer, J., A. van der Horst, and P. G. Wester. 2000. PBDEs and PBBd in suspended particulate matter, sediments, sewage treatment plant in- and effluents and biota from the Netherlands. Organohalogen Compounds 47:85-88.
De Carlo, V. J. 1979. Studies on brominated chemicals in the environment. Annals of the New York Academy of Sciences 320:678-681.
De Wit, C. A. 2002. An overview of brominated flame retardants in the environment. Chemosphere 46:583-624.
Egeler, P., J. Rombke, M. Meller, Th. Knacker, C. Franke, and G. Studinger. 1997. Bioaccumulation of lindane and hexachlorobenzene by tubificid sludgeworms (Oligochaeta) under standardised laboratory conitions. Chemosphere 35:835-852.
EHC. 1997. Brominated dipheny ethers. World Health Organization, 192, Geneva.
Fan, G., Y. Ouyang, and X. Xinlin. 1989. Reproduction and ontogenesis of Monopylephorus limosus. Journal of Zhejiang College of Fisheries 8:1-7.
Flores, F. J., and L. M. Tabche. 2001. The effects of chromium on the hemoglobin concentration of Limnodrilus hoffmeisteri (Oligochaeta: Tubificidae). Ecotoxicology and Environmental Safety 50:196-202.
Folk, R. L. 1966. A review of grain-size parameters. Sedimentology 6:73-93.
Forman, S., J. Kas, F. Fini, M. Steinberg, and T. Ruml. 1999. The effect of different solvents on the ATP/ADP content and growth properties of HeLa cells. Journal of biochemical molecular toxicology 13:11-15.
Gann, R. G. 1993. Flame retardants: overview. Pages 930-936 in Kirk-Othmer Encyclopedia of Chemical Technology, fourth edition. Wiley, New York.
Gillis, P. L., and T. B. Reynoldson, and D. G. Dixon. 2004. Natural variation in a metallothionein-like protein in Tubifex tubifex in the absence of metal exposure. Ecotoxicology and Environmental Safety 58:22-28.
Gorg, A., G. Boguth, O. Drews, A. Kopf, C. Luck, G. Reil, and W. Weiss. 2003. Two-dimensional electrophoresis with immobilized pH gradients for proteome analysis.
Gouin, T., and T. Harner. 2003. Modelling the environmental fate of the polybrominated diphenyl ethers. Environment International 29:717-724.
Gustafsson, K., M. Bjork, S. Burreau, and M. Gilek. 1999. Bioaccumulation kinetics of brominated flame retardants (polybrominated diphenyl ethers) in blue mussels (Mytilus edulis). Environmental Toxicology and Chemistry 18:1218-1224.
Hagmar, L., A. Sjodin, P. Hoglund, K. Thuresson, L. Rylander, and A. Bergman. 2000. Biological half-lives of polybrominated diphenyl ethers and tetrabromobisphenol A in exposed worders. Organohalogen Compounds 47:198-201.
Hale, R. C., M. J. La Guardia, E. Harvey, and T. M. Mainor. 2002. Potential role of fire retardant-treated polyurethane foam as a source of brominated diphenyl ethers to the US environment. Chemosphere 46:729-735.
Hale, R. C., M. Alaee, J. B. Manchester-Neesvig, H. M. Stapleton, and M. G. Ikonomou. 2003. Polybrominated diphenyl ether flame retardants in the North American environment. Environment International 29:771-779.
Hall, A. J., O. I. Kalantzi, and G. O. Thomas. 2003. Polybrominatd diphenyl ethers (PBDEs) in grey seals during their first year of life-are they thyroid hormone endocrine disrupters? Environmental Pollution 126:29-37.
Hallgren, S., T. Sinjari, and H. Hakansson. 2001. Effects of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) on thyroid hormone and vitamin A levels in rats and mice. Archives of Toxicology 75:200-208.
Hanberg, A., M. St_ahlberg, A. Georgellis, C. de Wit, U. G. Ahlborg. 1991. Swedish dioxin survey: evaluation of the H-4-II E bioassay for screening environmental samples for dioxin-like activity. Journal of Pharmacological and Toxicological Methods 69:442–449.
Hatai, S. 1898. On Vermiculus limosus, a new species of aquatic oligochaeta. Annot. Zool, Jpn. 2:103-111.
Hindersinn, R. R. 1990. Historical aspects of polymer fire retardance. Pages 415 in G. L. Nelson, editor. Fire and polymers hazard identification and prevention. American Chemical Society Symposium Series, New York.
Hites, R. A., J. A. Foran, S. J. Schwager, B. A. Knth, M. C. Hamiltion, and D. O. Carpenter. 2004. Global assessment of polybrominated diphenyl ethers in farmed and wild salmon. Environmental Science and Technology 38:4945-4949.
Hutzinger, O., G. Sundstrom, and S. Safe. 1976. Environmental chemistry of flame retardants. Part I. Introduction and principles. Chemosphere 1:3-10.
Hutzinger, O., and H. Thoma. 1987. Polybrominated dibezo-p-dioxins and dibenzofurans: the flame retardant issue. Chemosphere 16:1877-1880.
IRDC. 1974. Decabromodiphenyl ether. Acute toxicity studies in rats and rabbits. International Research and Development Corporation, Environmental Protection Agency.
IRDC. 1975. Octabromodiphenyl ether. Acute toxicity studies in rats and rabbits. International Research and Development Corporation, Environmental Protection Agency.
Jansson, B., R. Anderson, L. Asplund, K. Litzen, K. Nylund, U. Sellstrom, U. B. Uvemo, C. Wahlberg, U. Wideqvist, T. Odsjo, and M. Olsson. 1993. Chlorinated and brominated persistent organic compounds in biological samples from the environmental. Environmental Toxicology and Chemistry 12:1163-1174.
Jansson, B., L. Asplund, and M. Olsson. 1987. Brominated flame retardants - ubiquitous environmental pollutants? Chemosphere 16:2343-2349.
Klerks, P. L. 1987. Genetic adaptation to heavy metals in aquatic organisms: a review. Environmental Pollution 45:173-205.
Leppanen, M. T., and J. V. K. Kukkonen. 2004. Toxicokinetics of sediment-associated polybrominated diphenyl ethers (flame retardants) in benthic invertebrates (Lumbriculus variegatus, Oligochaeta). Environmental Toxicology and Chemistry 23:166-172.
Leynen, M., T.V. Berckt, J. M. Aerts, B. Castelein, D. Berckmans, and F. Ollevier. 1999. The use of Tubificidae in a biological early warning system. Environmental Pollution 105:151-154.
Madia, F., G. Giordano, V. Fattori, A. Vitalone, I. Branchi, F. Capone, and L.G. Costa. 2004. Differential in vitro neurotoxicity of the flame retardant PBDE-99 and of the PCB Aroclor 1254 in human astrocytoma cells. Toxicology Letters 154:11-21.
Madsen, T., S. Lee, and T. Olle. 2003. Growing threats: toxic flame retardants and children's health. Environment California Research and Policy Center, Los Angeles.
Martin, M., K. S. Lam, and B. J. Richardson. 2004. An Asian quandary : where have all of the PBDEs gone? Marine Pollution Bulletin 49:375-382.
Martinez, D. E., and J. Levinton. 1996. Adaptation to heavy metals in the aquatic oligochaete Limnodrilus hoffmeisteri: evidence for control by one gene. Evolution 50:1339-1343.
NICNAS. 2001. Polybrominated flame retardants (PBFRs). Priority existing chemical assessment report No. 20.
Norris, J. M., J. W. Ehrmantraut, C. J. Gibbons, R. J. Kocjba, B. A. Schwetz, J. Q. Rose, C. G. Humiston, G. L. Jewett, W.B. Crummett, P. L. Gehring, J. B. Tirsell, and J. S. Brosier. 1973. Toxicology and environmental factors involved in the selection of decabromodiphenyl oxide as a fire retardant chemical. Applied Polymer Symposium 22:195-219.
OECD. 2000. Risk assessment of diphenyl ether, pentabromo derivative (pentabromodiphenyl ether). SIDS initial assessment reprot.
Palm, A., I. T. Cousins, D. Mackay, M. Tysklind, C. Metcalfe, and M. Alaee. 2002. Assessing the environmental fate of chemicals of emerging concern: a case study of the polybrominated diphenyl ethers. Environmental Pollution 117:195-213.
Papke, O., L. Bathe, A. Bergman, P. Furst, D. M. Guvenius, and T. Herrmann. 2001. Determination of PBDEs in human milk from the United States-comparison of results from three laboratories. Organohalogen Compounds 52:197-200.
Peng, J. H. 2002. High-resolution gas chromatography-Mass spectrometric analysis for PBDD/PBDF/PBDE in environmental matrices. Master's Thesis. Chung Yuan Christian University, Chung Li.
Peters, A. J., P. Coleman, and K. C. Jpnes. 1999. Organochlorine pesticides in UK air. Organohalogen Compounds 41:447-450.
Rathore, R. S., and B. S. Khangarot. 2002. Effects of temperature on the sensitivity of sludg worm Tubifex tubifex to selected heavy metals. Ecotoxicology and Environmental Safety 53:27-36.
Rudel, R. A., D. E. Camann, J. D. Spengler, L. R. Korn, and J. G. Brody. 2003. Phthalates, Alkylphenols, Pesticides, Polybrominated Diphenyl Ethers, and Other Endocrine-Disrupting Compounds in Indoor Air and Dust. Environmental Science and Technology 37:4543-4553.
Ryan, J. J., B. Patry, P. Mills, and G. Beaudoin. 2002. Recent trends in levels of brominated diphenyl ethers (BDEs). Organohalogen Compounds 58:173-176.
Safe, S. 1994. Polychlorinated biphenyls (PCBs): environmental impact, biochemical and toxic responses, and implications for risk assessment. Toxicology 24:87-149.
Sanderson, J. T., J. M. M. J. G. Aarts, A. Brouwer, K. L. Froese, M. S. Denison, J. P. Giesy. 1996. Comparison of Ah receptor-mediated luciferase and ethoxyresorufin-O-deethylase induction in H4IIE cells: implications for their use as bioanalytical tools for the detection of polyhalogenated aromatic hydrocarbons. Toxicology and Applied Pharmacology 137:316–325.
Sellsrom, U., B. Jansson, A. Kierkegaard, C. de Wit, T. Odsio, and M. Olsson. 1993a. Polybrominated diphenyl ethers (PBDEs) in biological samples from the Swedish environment. Chemosphere 26:1703-1718.
Sellsrom, U., A. Kierkegaard, C. de Wit, B. Jansson, and M. Olss. 1993b. Time trend studies of polybrominated diphenyl ethers (PBDE) in biological samples from the Swedish environment. Chemosphere 14:211-213.
Sellstrom, U., A. Soderstrom, C. de Wit, and M. Tysklind. 1998. Photolytic debromination of decabromodiphenyl ether (DeBDE). Organohalogen Compounds 35:450-477.
Sellstrom, U., A. Kierkegaard, T. Alsberg, P. Jonsson, C. Wahlberg, and C. de Wit. 1999. Brominated flame retardants in sediments from European estuaries, the Baltic Sea and in sewage sludge. Organohalogen Compounds 40:383-386.
Sellstrom, U., and B. Jansson. 1995. Analysis of tetrabromobisphenol A in a product and environmental samples. Chemosphere 31:3085-3092.
Shepard, J. L., B. Olaaon, M. Tedengren, and B. P. Bradley. 2000. Protein expression signatures identified in Mytilus edulis exposed to PCBs, copper and salinity stress. marine Environmental Research 50:337-340.
Sjodin, A., K. Thuresson, L. Hagmar, E. Klasson-Wehler, and A. Bergman. 1996. Occupational exposure to polybrominated diphenyl ethers at dismantling of electronics - ambient air and human serum analysis. Organohalogen Compounds 43:447-450.
Sjodin, A., H. Carlsson, K. Thuresson, S. Sjolin, A. Bergman, and C. Ostman. 2001. Flame retardants in indoor air at an electronics recycling plant and at other work environments. Environmental Science and Technology 35:448-454.
Sjodin, A., D. G. Patterson Jr, and A. Bergman. 2003. A review on human exposure to brominated flame retardants - particularly polybrominated diphenyl ethers. Environment International 29:829-839.
Sjodin, A. L. H., E. Klasson-Wehler, J. Bjork, and A. Bergman. 2000. Influence of the consumption of fatty Baltic Sea fish on plasma levels of halogenated environmental contaminants in Latvian and Swedish men. Environmental Health Perspectives 35:448-454.
Smital, T., R. Sauerborn, and B.K. Hackenberger. 2003. Inducibility of the P-glycoprotein transport activity in the marine mussel Mytilus galloprovincialis and the freshwater mussel Dreissena polymorpha. Aquatic Toxicology 65:443-465.
Strandberg, B., N. Dodder, I. Basu, and R. Hites. 2001. Concentrations and spatial variations of polybrominated diphenyl ethers and other organohalogen compounds in Great Lakes air. Environmental Science and Technology 35:1078-1083.
Thomsen, C., E. Lundanes, and G. Becher. 2002. Brominated flame retardants in archived serum samples from Norway: a study on temporal trends and the role of age. Environmental Science and Technology 36:1414-1418.
Tullo, A. H. 2000. Plastic additives steady evolution. Chemical and Engineering News 78:49.
Ueno, D., N. Kajiwara, H. Tanaka, A. Subramanian, G. Fillmann, K. S. Lam, G. J. Zheng, M. Muchitar, H. Razak, M. Prudente, K. H. Chung, and S. Tanabe. 2004. Global pollution monitoring of polybrominated diphenyl ethers using skipjack tuna as a bioindicator. Environmental Science and Technology 38:2312-2316.
Viarengo, A., M. N. Moore, G. Mancinelli, A. Mazzucotelli, R. K. Pipe, and S. V. Farrar. 1987. Metallothioneins and lysosomes in metal toxicity and accumulation in marine mussels: the effects of cadmium in the presence and absence of phenanthrene. Marine Biology 94:251-257.
Viberg, H., A. Fredriksson, and P. Eriksson. 2003. Neonatal exposure to polybrominated diphenyl ether (PBDE 153) disrupts spontaneous behaviour, impairs learning and memory, and decreases hippocampal cholinergic receptors in adult mice. Toxicological and Applied Pharmacology 192:95-106.
Wallace, W. G., G. R. Lopez, and J. S. Levintion. 1998. Cadmium resistance in an oligochaete and its effect on cadmium trophic transfer to an omnivorous shrimp. Marine Ecology Progress Series 172:225-237.
Wania, F., and C. Dugani. 2003. Assessing the long-range transport potential of polybrominated diphenyl ethers: a comparison of four multimedia models. Environmental Toxicology and Chemistry 22:1252-1261.
Watanabe, I., M. Kawano, Y. Wang, Y. Chen, and R. Tatsukawa. 1992. Polybrominated dibenzo-p-dioxins (PBDDs) and - dibenzofurans (PBDFs) in atmospheric air in Taiwan and Japan. Organohalogen Compounds 9:309-312.
Westermeier, R., and T. Naven. 2002. Proteomics in practice: a laboratory manual of proteome analysis. Electrophoresis in practice. Wiley-VCH, Weinheim.
Zhou, T., M. M. Taylor, M. J. de Vito, and K. M. Crofton. 2002. Developmental exposure to brominated diphenyl ethers results in thyroid hormone disruption. Toxicological Sciences 66:105-116.
Zitko, V. 1993. Expanded polystyrene as a source of contaminants. Marine Pollution Bulletin 26:584-585.