跳到主要內容

臺灣博碩士論文加值系統

(44.222.131.239) 您好!臺灣時間:2024/09/09 20:01
字體大小: 字級放大   字級縮小   預設字形  
回查詢結果 :::

詳目顯示

: 
twitterline
研究生:黃思瑀
研究生(外文):Sih-yu Huang
論文名稱:河川底泥多氯聯苯污染之調查與復育規劃
論文名稱(外文):Investigation of PCBs contaminated sediments and bioremediation in river
指導教授:錢紀銘錢紀銘引用關係
指導教授(外文):Ji-ming Cian
學位類別:碩士
校院名稱:嘉南藥理科技大學
系所名稱:環境工程與科學系碩士班
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2006
畢業學年度:94
語文別:中文
論文頁數:98
中文關鍵詞:SABAroclors多氯聯苯脫氯作用
外文關鍵詞:SABpolychlorinated biphenylsdechlorinationAroclors
相關次數:
  • 被引用被引用:5
  • 點閱點閱:382
  • 評分評分:
  • 下載下載:63
  • 收藏至我的研究室書目清單書目收藏:0
本研究採集南台灣二仁溪下流流域之底泥6處,將採得之底泥分為表層底泥(0~30 公分)及深層底泥(31~60 公分),針對不同深度之底泥進行多氯聯苯含量分析調查,A點表層底泥(0~30 公分)全部多氯聯苯濃度總合為4.814 μM,其中以2,3,6,3'',4''-CBp 15.25%佔的百分比最多,次之是2,4,3'',4''-CBp 13.74%及2,4,5,3'',4''-CBp之13.47%。 A點深層底泥(31~60 公分)全部多氯聯苯濃度總合為1.676 μM,其中以23452''3''4''-CBp, 38.89%佔的百分比最多。B、C兩點表層底泥(0~30 公分)及深層底泥(31~60 公分)並無出現任何多氯聯苯。D點表層底泥(0~30 公分)以253''5''-CBp, 12.41%所佔百分比最高,252''-CBp, 11.76%次之。D點深層底泥(31~60 公分)以23452''3''4''-CBp, 26.20%所佔百分比最高,其次是242''5''- CBp, 15.74%。E點表層底泥(0~30 公分)以262''-CBp, 47.31%所佔百分比最高,其次是23452''3''4''-CBp, 25.25%。E點深層底泥(31~60 公分)以252''-CBp, 17.62%所佔百分比最高,其次是253''5''-CBp, 12.07%。F點表層底泥(0~30 公分)以23452''3''4''-CBp, 93.19%所佔百分比最高,而F點深層底泥(31~60 公分), 23452''3''4''-CBp, 21.69%所佔百分比最高,其次是252''-CBp, 7.85%;各點之污染狀況與Aroclor 1242近似,皆有較低氯數之多氯聯苯的存在。
此外本研究建立模擬箱模擬環境中多氯聯苯之脫氯情形,土壤管柱中添加234-CBp、253''4''-CBp、242''5''-CBp、2452''4''5''-CBp及Aroclor 1242,經過3個月的置放培養後,發現234-CBp濃度皆有降低的現象;也發現有24-CBp的脫氯產物,證實模擬箱中234-CBp管柱中有明顯的脫氯作用存在。253''4''-CBp及242''5''-CBp濃度皆有降低的現象;而在253''4''-CBp發現在11~15cm及21~25cm有342''-CBp的脫氯產物,242''5''-CBp之管柱也發現在16~20cm有24''-CBp, 0.1415 μM及發現252''-CBp, 1.1745 μM的脫氯產物。
2,4,5,2'',4'',5''-CBp發現有部分242''5''-CBp、242''4''-CBp、2,4,5,2'',5''-CBp及2,4,5,2'',4''-CBp脫氯產物,因此2,4,5,2'',4'',5''-CBp應有脫氯作用的發生。
In order to investigate polychlorinated biphenyls (PCBs) contamination in the river sediment in southern Taiwan, every 2 layers (the upper layer 0 ~ 30 cm, and the lower layer 30 ~ 60 cm, in depth) of sediments from 6 different sites were collected and analyzed the PCBs content. The results showed that in the upper layer of Site A, total PCBs concentration was 4.814 �嵱, 2,3,6,3’,4’-chlorobiphenyl (2,3,6,3’,4’-CB) was the most abundant congeners with a ratio of 15.25 %, and 2,4,3’,4’-CB and 2,4,5,3’,4’-CB were 13.74 %, 13.47 %, respectively. In site B and site C, there was no significant PCBs contamination. In Site D upper layer, 2,5,3’,5’-CB and 2,5,2’-CB were the major congeners with 12.41% and 11.76 % of weight ratio. Similar to the lower layer of Site E, 2,5,2’-CB and 2,5,3’,5’-CB were two most abundant congeners. However, in Site F lower layer, 2,3,4,5,2’,3’,4’-CB was congeners with the highest concentration of 21.69%, then 252''-CBp was of 7.85%. Except Site F lower layer, most of the layers with significant PCBs contamination showed the similar congener distribution with Aroclor 1242.
While the investigation of PCBs contamination was completed, a Simulated Aquarium Box (SAB) was constructed in a purpose of evaluating PCBs dechlorination in natural sediment environment. Sediment columns amended with different PCBs congeners or mixture such as 2,3,4-CB, 2,5,3’,4’,-CB, 2,4,2’,5’-CB 2,4,5,2’,4’,5’-CB and Aroclor 1242 were introduced into SAB for PCBs dechlorination tests. After 3 months of incubation, 2,3,4-CB concentration decreased and 2,4-CB was found. It suggested that PCBs dechlorination happened in the sediment. In 2,5,3’,4’-CB and 2,4,2’,5’-CB columns, the concentration were both decreasing, and their dechlorination products, 3,4,2’-CB and 2,5,2’-CB were also produced. 2,4,5,2’,4’,5’-CB, a congener with 6 substituted chlorines was thought not easily dechlorinated, however in SAB, it’s dechlorination product such as 2,4,2’,4’-CB, 2,4,2’,5’-CB and 2,4,5,2’,4’-CB, 2,4,5,2’,5’-CB were produced during a 3 months of incubation.
目錄
摘要 I
英文摘要 III
致謝 V
目錄 VI
表目錄 VIII
圖目錄 X
一、前言 1
1.1研究緣起 1
1.2研究目的 5
二、文獻回顧 9
三、研究方法 19
3.1實驗材料 19
3.1.1藥品 19
3.1.2儀器設備 22
3.2方法及步驟 23
3.2.1多氯聯苯同類物的鑑定方法的建立 24
3.2.1.1多氯聯苯同類物定性分析方法步驟 24
3.2.1.2多氯聯苯同類物定量分析方法步驟 26
3.2.2二仁溪底泥中多氯聯苯調查實驗流程 27
3.2.2.1底泥採樣 28
3.2.2.2底泥萃取步驟 31
3.2.2.3多氯聯苯之GC分析條件 32
3.2.3建立模擬箱模擬環境中PCBs之脫氯實驗 33
3.2.3.1建立模擬箱模擬環境中PCBs之實驗規劃流程 33
3.2.3.2河水萃取步驟 35
3.2.4二仁溪底泥多孔性通透管柱之埋設實驗 36
3.2.4.1多孔性通透管柱埋設實驗流程 36
3.2.4.2多孔性通透管柱埋設實驗步驟 37
四、結果與討論 40
4.1多氯聯苯鑑定分析方法之建立 40
4.2二仁溪底泥中多氯聯苯濃度調查情況 49
4.3以模擬箱模擬環境中PCBs之實驗建立過程 60
4.4模擬箱實驗之初步結果 64
五、結論與建議 73
六、參考文獻 75
附錄I 1997年陳意銘GC分析所得之多氯聯苯同類物之層析數據 82


表目錄
表一 各種多氯聯苯經厭氧微生物還原脫氯作用後之脫氯型態 8
表二 22種多氯聯苯單品同類物 20
表三 PCB Calibration Check Solution之同類物 21
表四 二仁溪底泥採樣座標位置 30
表五 本研究GC分析之多氯聯苯同類物滯留時間 41
表六 本研究GC分析所得之多氯聯苯同類物之層析數據 42
表七 國外河川底泥中多氯聯苯含量(37) 52
表八 本研究A、B點不同深度底泥,以GC分析所得之多氯聯苯同類物濃度 53
表九 本研究C、D點不同深度,以GC分析所得之多氯聯苯同類物 56
表十 本研究E、F點不同深度之底泥,以GC分析所得之多氯聯苯同類物 59
表十一 填充管柱添加之氯苯化合物及濃度 60
表十二 模擬箱管柱中多氯聯苯最初添加之PCBs之濃度 66
表十三 模擬箱管柱中2,3,4-CBpb在不同深度下出現的多氯聯苯濃度 68
表十四 模擬箱管柱中2,5,3'',4''-CBpb在不同深度下出現的多氯聯苯濃度 68
表十五 模擬箱管柱中2,4,2'',5''-CBpb在不同深度下出現的多氯聯苯濃度 69
表十六 模擬箱管柱中2,4,5,2'',4'',5''-CBpb在不同深度下出現之多氯聯苯濃 度 69
表十七 模擬箱管柱中Aroclor 1242b在不同深度下出現的多氯聯苯濃度 70
表十八 模擬箱ORP監測值 72


圖目錄
圖一 二仁溪底泥中多氯聯苯調查實驗流程圖 27
圖二 本研究二仁溪底泥採樣位置圖 29
圖三 徐明豐研究採樣位置圖 29
圖四 建立水槽箱模擬環境中PCBs之實驗規劃流程圖 33
圖五 槽體水循環系統建立圖 34
圖六 模擬槽內部管柱示意圖 34
圖七 多孔性通透管柱埋設實驗流程圖 36
圖八 PVC材質之多孔性通透管柱 38
圖九 至河岸邊挖出約 0.5*0.5*0.7 公尺之埋管洞 38
圖十 將裡土裝入箱子內,攪拌箱子內的裡土使其均勻 38
圖十一 裡土分別填滿至三支管柱內 39
圖十二 三支管柱填入混合後之底泥置入埋管洞,並作記號 39
圖十三 箱內其餘之裡土回填至埋管洞內 39
圖十四 底泥槽及河水槽,槽體體積長 90cm寬 45cm高 45cm 62
圖十五 填充過後之28根管柱平均置放於底泥槽中 62
圖十六 底泥層上再加入二仁溪河水5 cm高 62
圖十七 河水槽加入二仁溪河水35 cm高 63
圖十八 底泥槽、河水槽以導管相通並以電動幫浦驅動水流 63
圖十九 模擬箱完成圖 63
六、參考文獻
1.Quensen, J.F.Ⅲ, J.M. Tiedje S.A. Boyd.“Reductive dechlorination of polychlorinated biphenyls by Anaerobic microorganisms from sediments. ”, Science. 242: 752-754. 1988.
2.Schmidt, H. and Schultz, G. Ann. Chem., 207:338. 1881.
3.Juergen Wiegel., Qingzhong Wu. “Microbial reductive dehalogention of polychlorinated biphenyls.”, FEMS Microbology Ecology. 32:1-15. 2000.
4.Brown Jr., J.F., R.E. Wagner, H. Feng, D.L.Bedard, M.J. Brennan, J.C. Carnahan, R.J. “Environmental dechlorination of PCBs. Environ.”, Toxicol. Chem. 6: 579-593. May. 1987.
5.羅初英, 多氯聯苯、戴奧辛等有機氯化物在土壤及水質中含量分析, 行政院國家科學委員會環保大型計畫, 二仁溪污染大型研究計畫 NSC78-0421-e-006-18-z,1989。
6.郁仁貽,環境污染防治,復文書局,1988。
7.Milling A., W.F. Müller, F. Coulston amd F. Korte. “Comparative metabolism of 2,2’-dichlorobiphenyl-14C in mice, rats, and monkeys after single oral application.”, Chemosphere. 8:15-19. 1979.
8.Torok et al. “Delayed pregnancy in NMRI mice treated with PCB:2,2’-dichlorobiphenyl.”, Bull. Environ. Contam. Toxicol. 16:33-36. 1976.
9.Freitag D., M. Hass-Jobelius and Yin Yiwei. “Influence of 2,2’- dichlorobiphenyl and 2,4,6-trichlorophenol on development of rainbow trout eggs and larvae.”, Toxico. Envir. Chem. 31.32:401-408. 1991.
10.Waid J., S. D. Phil and F.I. Biol. “PCBs and the environment Volume Ⅲ”,p27-38. 1986.
11.Jeremiason, J.D. K.C. Hornbuckle, and S.J. Eisenreich. “PCBs in Lake Superior, 1978-1992:decreases in water concentrations reflect loss by volatilization.”, 28:903-914. 1994.
12.Bedard, D.L., R.E. Wagner, M.J. Brennan, M.L. Haberl and J.F. Brown. “Extensive degradation of Aroclors and environmentally transformed polychlorinated biphenyls by Alcaligenes eutrophus H850.”, Appl. Environ. Microbiol. 53: 1094-1102. 1987.
13.Brown, J.F., D.L. Bedard, M.J. Brennan, J.C. Carnahan, H. Feng and R.E. Wagner. “Polychlorinated biphenyl dechlorination in aquatic sediments. ”, Science. 236: 709-712. 1987.
14.Lajoie, C.A., A.C. Layton and G.S. Sayler. “Cometabolic oxidation of polychlorinated biphenyls in soil with a surfactant-based field application vector.”, Appl.Environ. Microbiol.60: 2826-2833. 1994.
15.Mondello, F.J. “Cloning and expression in Escherichia coli of Pseudomonas strain LB400 genes encoding polychlorinated biphenyl degradation.”, J. Bacteriol.171: 1725-1732. 1989.
16.陳意銘,馴化厭氧菌對六氯苯還原性脫氯作用影響因子之探討,東吳大學微生物研究所碩士論文,p.85, 1994。
17.陳意銘,台灣本土厭氧菌對多氯聯苯還原性脫氯作用之研究,台灣大學農業化學研究所博士論文,1997。
18.Brown Jr., J.F., R.E. Wagner, H. Feng, D.L.Bedard, M.J. Brennan, J.C. Carnahan and R.J. “Environmental dechlorination of PCBs. Environ.”, Toxicol. Chem. 6: 579-593. May.1987.
19.Alder, A.C., M.M.Haggblom, S.R.Oppenheimer and L.Y.Young. “Reductive dechlorination of polychlorinated biphenyls in anaerobic sediments.”, Environ. Sci. Technol. 27: 530-538. 1993.
20.Mohn, W.W. and J.M. Tiedje. “Microbial reductive Dehalogenation. Microbiol.”, Rev. 56: 482-507. 1992.
21.Eisenreich S.J., B.B. Looney and JD. Thornton. “Airborne organic contaminants in the Great Lakes ecosystem.”, Environ Sci Technol. 15:30-38. 1981.
22.Karickhoff SW. “Organic pollutant sorption in aquatic systems.”, J. Hyd. Engr. 110:707-735. 1984.
23.Steen W.C., D.F. Paris amd G.L. Baughman. “Partitioning of selected polychlorinated biphenyls to natural sediments.”, Water Res. 12:655-657. 1978.
24.Frank M. Dunnivant, Anne L. Polansky and Alan W. Elzerman. “Persistence and distribution of PCBs in the sediments of a reservoir(Lake Hartwell, South Carolina).”, Bull. Environ. Contam. Toxicol. 43:870-878. 1989.
25.Thomas R. L., J. P. Vernet and R. Rrank. “ΣDDT, PCBs, and HCB in the sediments of Lake Geneva and the Upper Rhône River.”, Environmental Geology. 5:103-113. 1984.
26.Rhee, G.Y., R.C.Sokol, C.M. Bethoney and B. Bush. “Dechlorination of polychlorinated biphenyls by Hudson River Sediment organisms: Specificity to the chlorination pattern of congeners.”, Environ. Sci. Technol. 27: 1190-1192. 1993.
27.Bernal J. L., Jesús Del Nozal M., L. Toribio and J. Brogeras “Polychloinated Biphenyl analysis in sediments from castile and leon reservoirs.”, Toxic. Envir. Chem. 35:137-148. 1992.
28.Kalajzic T., M. Bianchi, H. Muntau and A. Kettrup. “Polychlorinated biphenyls(PCBs) and organochlorine pesticides(OCPs) in the sediments of an italian drinking water reservoir.”, Chemosphere. 36:1615-1625. 1998.
29.Mangani F., G. Crescentini, E. Sisti and F. Bruner. ,“PAHs, PCBs and chlorinated pesticidies in mediterraneal coastal sediments.” 45:89-100. 1991.
30.Hutzinger, O., S. Safe, and V. Zitko. “The Chemistry of PCBs, CRC Press, Cleveland. ” 1974.
31.Richard F. Bopp, H. James Simpson, Curtis R. Olsen, Robert M. Trier, and Nadia Kostyk. “Chlorinated hydrocarbons and radionuclide chronologies in sediments of the Hudson River and estuary, New York.”, Environ. Sci. Technol. 16:668-676. 1982.
32.Bush B., L. A. Shane, M.Wahlen and Mark P. Brown. “Sedimentation of 74 PCB congeners in the upper Hudsion River.”, Chemosphere. 16:733-744. 1987.
33.William P. Flanagan and Ralph J. May. “Metabolite detection as evidence for naturally occurring aerobic PCB biodegradation in Hudson River sediments.”, Environ. Sci. Technol. 27:2207-2212. 1993.
34.Chevreuil M., M. Blanchard, M. J. Teul and A. “Chesterikoff. Polychlorobiphenyl behaviour in the water/sediment system of the Seine river, France.”, Wat. Res. 32:1204-1212. 1998.
35.翁鎮聖,台灣近河口多氯聯苯污染含量分析之研究,私立中原大學化學研究所碩士論文,1994。
36.胡安仁,二仁溪流域河床淤泥及兩岸土壤中多氯聯苯含量分析,國立成奶j學碩士論文,1991。
37.徐民豐,二仁溪河川底泥性質與多氯聯苯分佈狀況之研究,國立臺灣大學碩士論文,1998。
38.王一雄、陳尊賢、李達源, 有機污染物來源與特性, 土壤污染學, 國立空中大學出版,1995。
39.Quensen, J.F.Ⅲ, S.A. Boyd and J.M. Tiedje. “Dechlorination of four commercial polychlorinated biphenyl mixtures (Aroclors) by anaerobic microorganisms from sediments.”, Appl. Environ. microbiol.56: 2360-2369. 1990.
40.Bopp RF., H.J. Simpson, Olsen CR., and Kostyk N. “PCBs in sediment of the tidal Hudson River, New York.”, Environ. Sci. Technol. 15:210-216. 1981.
41.Morris, P.J., W.W. Mohn, J.F. Quensen Ⅲ, J.M. Tiedje and S.A. Boyd. “Establishment of a polychlorinated biphenyl-degrading enrichment culture with predominantly meta dechlorination.”, Appl. Environ. Microbiol. 58: 3088-3094. 1992.
42.Rhee, G.Y., R.C.Sokol, C.M. Bethoney and B. Bush. “Dechlorination of polychlorinated biphenyls by Hudson River Sediment organisms: Specificity to the chlorination pattern of congeners.”, Environ. Sci. Technol. 27: 1190-1192. 1993.
43.Bryant, F.O., D.H. Hale and J.E. Rogers. “Regiospecific dechlorination of pentachlorophenol by dichlorophenol-adapted microorganisms in fresh water, anaerobic sediment slurries.”, Appl. Environ. Microbiol. 57: 2293-2301. 1991.
44.Rhee, G.Y., R.C. Sokol, C.M. Bethoney and B. Bush. “A long term study of anaerobic dechlorination of PCB congerners by sediment microorganisms: pathway and mass balance.”, Environ.Toxicol.Chem. 12: 1829-1835. 1993.
45.Williams W.A. “Microlbial reductive dechlorination of trichlorophenyls on anaerobic sediment sluuries.”, Environ.Sci. Technol. 28: 630-635. 1994.
46.Qingzhong Wu., Kevin R. Sowers., Harold D. May. “Microbial reductive dechlorination of Aroclor 1260 in anaerobic slurries of estuarine sediments.”, Appl. Environ. Microbiol. 64: 1052-1058. 1998.
47.I-Ming Chen. “PCB-dechlorination capability of sediment microbes in Erh-Jen river.”, Environmental Polloution Control Technology. P.1-9. 2004.
48.Nicholson, D. K., S. L. Woods, J. D. Istok, and D. C. Peek. “Reductive dechlorination of chlorophenols by a pentachlorophenolacclimated methanogenic consortium.”, Appl. Environ. Microbiol. 58:2280-2286. 1992.
49.Mikesell, M. D., and S. A. Boyd. “Complete reductive dechlorination and mineralization of pentachlorophenol by anaerobic microorganisms.”, Appl. Environ. Microbiol. 52: 861-865. 1986.
50.Pavoni B., Duzzin B. and Donazzolo R. “Contamination by chlorinated hydrocarbons (DDT, PCBs) in surface sediment and macrobenthos of the river Adige(Italy).”, The Science of the Total Environment. 160:1-17. 1987.
51.Smit Z., V. DrevenKar and M. Kodrie-Smit. “Polychlorinated biphenyls in the Kupa river, Croatia, Yugoslavia.”, Chemosphere. 16:2351-2358. 1987.
52.Terytze K. “Low volatile chlorinated hydrocarbons and heavy metals in aquatic sediments in Berlin and envurons. Intern.”, J. Environ. Anal. Chem. 59:197-211. 1995.
53.Passivists J., K. Häntykoski, R. Paukhu, T. Piilola, H. Vihonea, J. Särkhä and K. Granberg. “PCB in the sediment of the lake Jyväsjärvi.”, Aqua Fennica. 16:17-23. 1986.
54.Thomas R. L., J. P. Vernet and R. Rrank. “ΣDDT, PCBs, and HCB in the sediments of Lake Geneva and the Upper Rhône River.”, Environmental Geology. 5:103-113. 1984.
55.Thomas R. L. and R. Rrank. “Trends in organic pollutants in Lake Ontario sediments 1968-1987.”, Eclogae geol. Helv. 87:403-407. 1994.
56.Chevreuil M., M. Blanchard, M. J. Teul and A. Chesterikoff. “Polychlorobiphenyl behaviour in the water/sediment system of the Seine river, France.”, Wat. Res. 32:1204-1212. 1998.
QRCODE
 
 
 
 
 
                                                                                                                                                                                                                                                                                                                                                                                                               
第一頁 上一頁 下一頁 最後一頁 top
無相關期刊