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研究生:徐明聖
研究生(外文):HSU Ming Sheng
論文名稱:台灣地區戴奧辛類化合物膳食攝入量調查及其健康風險評估
論文名稱(外文):Investigation of Dietary Intake in Taiwan for Dioxin-like Compounds and its Health Risk Assessment
指導教授:凌永健凌永健引用關係
指導教授(外文):LING Yong Chien
學位類別:博士
校院名稱:國立清華大學
系所名稱:化學系
學門:自然科學學門
學類:化學學類
論文種類:學術論文
論文出版年:2004
畢業學年度:92
語文別:中文
中文關鍵詞:戴奧辛戴奧辛類多氯聯苯戴奧辛類化合物膳食攝入量健康風險食品
外文關鍵詞:dioxindioxin-like PCBsdioxin like compoundsdietary intakehealth riskfood
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本研究採用選擇研究個別食品方式以估算台灣地區民眾之膳食戴奧辛類化合物(dioxin-like compounds, DLCs)攝入量,並進行健康風險評估。本研究於2000年~2003年間,在台灣地區共採集市售3477件動物來源或高脂食品樣品,經混樣後得到380件組合樣品,分析其中的17種2,3,7,8-氯取代戴奧辛/呋喃化合物。在調查的22類食品中,總重基準上界平均戴奧辛濃度介於0.020~0.255 pg WHO-TEQPCDD/F/g fw,而脂肪重基準上界平均戴奧辛濃度則介於0.179~3.74 pg WHO-TEQPCDD/F/g lw。此外,本研究亦藉由測定部份牛肉、魚肉與全脂牛乳樣品中12種戴奧辛類多氯聯苯的濃度,推估陸生與水生動物來源食品中戴奧辛與戴奧辛類多氯聯苯的毒性當量(toxicity equivalency quantity, TEQ)比例,陸生動物食品:戴奧辛佔65% TEQ,戴奧辛類多氯聯苯佔35% TEQ;水生動物食品:戴奧辛佔35% TEQ,戴奧辛類多氯聯苯佔65% TEQ。
台灣地區成年男女的膳食DLCs攝入量經估算後,一般族群(50th percentile)介於0.6~0.8 pg WHO-TEQPCDD/F+PCB/kg bw/day,第95百分位族群(95th percentile)介於2.2~3.0 pg WHO-TEQPCDD/F+PCB/kg bw/day,魚類食品為主要的膳食DLCs TEQ來源,有近50%的TEQ貢獻;肉類食品為次要的膳食DLCs攝入來源,約佔35%的TEQ貢獻;乳製品類、蛋類與油脂類食品的TEQ貢獻比例相當,各約佔5%。以世界衛生組織(World Health Organization, WHO)於 1998年提出的DLCs日容許攝入量(tolerable daily intake, TDI)建議值1~4 pg WHO-TEQPCDD/F+PCB/kg bw/day做為健康風險評估依據時,即使加上未被納入調查的植物性食品之TEQ貢獻,DLCs可能引起致癌與非致癌效應的健康風險仍是在可接受的範圍內。
This study uses the approach of selective studies of individual foods to investigate the dietary intake of dioxin-like compounds by Taiwanese from 2000 to 2003. The concentrations of seventeen 2,3,7,8-substituted polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) are measured in a total of 380 compound samples, assembled from 3477 individual food samples of animal origin and high fat, are measured. Furthermore, twelve dioxin-like PCBs in some beef, milk and fish samples are also measured to evaluate their contributions of toxicity equivalency quantity (TEQ) between terrestrial and aquatic animal foods. The upper bound average concentrations of PCDD/DFs in 22 classes of foods investigated in this study range from 0.020 to 0.255 pg WHO-TEQPCDD/F /g on fresh weight basis, or from 0.179 to 3.74 pg WHO-TEQPCDD/F /g on lipid basis. The estimated TEQ contributions from dioxin-like PCBs are 35% and 65% of total TEQ in terrestrial and aquatic animal foods, respectively.
The upper bound dietary intakes of DLCs among the general population (50th percentile) of Taiwanese adults are calculated in the range of 0.6~0.8 pg WHO-TEQPCDD/F+PCB/kg bw/day, and 2.2~3.0 pg WHO-TEQPCDD/F+PCB/kg bw/day for the 95th percentile population. Fish meats are regarded as the principal dietary source of DLCs intake, approximately contributing to half of dietary intake of DLCs. Terrestrial meats are the secondary TEQ contributors and estimate to have 35% contribution. Dairy products, eggs and oil/fat foods contribute only ca. 5% of dietary intake of DLCs each.
The average daily intake of DLCs from foods of animal origin and high fat for the general population of Taiwanese adults is within the tolerable daily intake (TDI), i.e., 1-4 pg WHO-TEQ/kg bw/day, recommended by World Health Organization in 1998. If the TEQ contributions from foods of plant origin are also taken into consideration, the human health risks of cancer and non-cancer effects by the current dietary intake of DLCs by Taiwanese adults are still acceptable.
Chapter 1
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Chapter 2
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24. 台南縣政府主計室,統計月報http://intranet.tnhg.gov.tw/files/tnhg/A17/dept4/month_papers/93_5.xls
25. 高雄市區里人口統計資料查詢系統http://cabu.kcg.gov.tw/people/92r3110.htm
26. 高雄縣民政局,現住戶數、人口密度及性比例,1222-01-01-2。
27. Liem, A. K. D. (1999). Basic aspects of methods for the determination of dioxins and PCBs in foodstuffs and human tissues, Trends in Analytical Chemistry, 18, 429-439.
28. AOAC Official Methods of Analysis 970.52L(c) “Fat-Containing Foods”, 15th Ed. 1990, 278-279.
29. Ryan, J. J.; Lizotte, R.; Panopio, L. G.; Lau, B. P. Y. (1989). The effect of strong alkali on the determination of polychlorinated dibenzofurans (PCDFs) and polychlorinated dibenzo-p-dioxins (PCDDs), Chemosphere, 18, 149-154.
30. US EPA Method 1613B (1994). Tetra- through Octa-Chlorinated Dioxins and Furans by Isotope Dilution HRGC/HRMS, US EPA.
31. Malisch, R.; Schmid, P.; Frommberger, R.; Fürst, P. (1996). Results of a quality control study of different analytical methods for determination of PCDD/PCDF in egg samples, Chemosphere, 32, 31-44.
32. Strandberg, B.; Bergqvist. P. A.; Rappe, C. (1998). Dialysis with semipermeable membranes as an efficient lipid removal method in the analysis of bioaccumulative chemicals, Analytical Chemistry, 70, 526-533.

33. Grochowalski, A.; Chrzaszcz, R. (2000). The result of the large scale determination of PCDDs, PCDFs and coplanar PCBs in polish food product samples using GC-MS/MS technique, Organohalogen Compounds, 47, 310-313.
34. Smith, L. M.; Stalling, D. L.; Johnson, J. L. (1984). Determination of part-per-trillion levels of polychlorinated dibenzofurans and dioxins in environmental samples, Analytical Chemistry, 56, 1830-1842.
35. Liem, A. K. D.; de Jong, A. P. J. M.; Marsman, J. A.; den Boer, A. C.; Groenemeijer, G. S.; den Hartog, R. S.; de Korte, G. A. L.; Hoogerbrugge, R.; Kootstra, P. R.; van’t Klooster, H. A. (1990). A rapid clean-up procedure for the analysis of polychlorinated dibenzo-p-dioxins and dibenzofurans in milk samples, Chemosphere 1990, 20, 843-850.
36. Krokos, F.; Creaser, C. S.; Wright, C.; Startin, J. R. (1997). Congener-specific method for the determination of ortho and non-ortho polychlorinated biphenyls, polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans in foods by carbon-column fractionation and gas chromatography-isotope dilution mass spectrometry, Fresenius Journal of Analytical Chemistry, 357, 732-742.
37. Reiner, E. J.; Schellenberg, D. H.; Taguchi, V. Y.; Mercer, R. S.; Townsend, J. A.; Thompson, T. S.; Clement, R. E. (1990). Application of tandem quadrupole mass spectrometry for the ultra-trace determination of polychlorinated dibenzo-p-dioxins and dibenzofurans, Chemosphere, 20, 1385-1392.
38. Hayward, D. G. (1997). Determination of polychlorinated dibenzo-p-dioxin and dibenzofuran background in milk and cheese by quadrupole ion storage collision induced dissociation MS/MS, Chemosphere, 34, 929-939.
39. Hayward, D. G.; Hooper, K.; Andrzejewski, D. (1999). Tandem-in-time mass spectrometry method for the sub-parts-per-trillion determination of 2,3,7,8-chlorine-substituted dibenzo-p-dioxins and –furans in high-fat foods, Analytical Chemistry, 71, 212-220.

40. Hayward, D. G.; Holcomb, J.; Glidden, R.; Wilson, P.; Harris, M.; Spencer, V. (2001). Quadrupole ion storage tandem mass spectrometry and high-resolution mass spectrometry: complementary application in the measurement of 2,3,7,8-chlorine substituted dibenzo-p-dioxins and dibenzofurans in US foods, Chemosphere, 43, 407-415.
41. Ferrario, J.; Byrne, C.; McDaniel, D.; Dupuy, A. Jr. (1996). Determination of 2,3,7,8-chlorine-substituted dibenzo-p-dioxins and furans at the part per trillion level in United States beef fat using high-resolution gas chromatography / high-resolution mass spectrometry, Analytical Chemistry, 68, 647-652.
42. Schecter, A.; Cramer, P.; Boggess, K.; Stanley, J.; Olson, J. R. (1997). Levels of dioxins, dibenzofurans, PCB and DDE congeners in pooled food samples collected in 1995 at supermarkets across the United States, Chemosphere, 34, 1437-1447.
43. US FDA Laboratory Information Bulletin No. 4084 Dioxins (1997). “Quadrupole Ion Storage Mass Spectrometry/Mass Spectrometry Application to the Analysis of all 17 2,3,7,8 substituted Chlorodibenzo-p-dioxins (dioxins) and Chlorodibenzofurans (furans) in Dairy Products and High Fat Foods”
44. Harrison, N.; Wearne, S.; Gem, M. G. de M.; Gleadle, A.; Startin, J.; Thorpe, S.; Wright, C.; Kelly, M.; Robinson, C.; White, S.; Hardy, D.; Edinburgh, V. (1998). Time trends in human dietary exposure to PCDDs, PCDFs and PCBs in the UK, Chemosphere, 37, 1657-1670.
45. Ryan, J. J.; Mills, P. (1997). Lipid extraction from blood and biological samples and concentrations of dioxin-like compounds, Chemosphere, 34, 999-1009.
46. Malisch, R. (1998). Update of PCDD/PCDF-Intake from food in Germany, Chemosphere, 37, 1687-1698.
47. Schecter, A.; Päpke, O.; Dellarco, M.; Olson, J. (1996). A comparison of dioxins and dibenzofurans in cooked and uncooked food, Organohalogen Compounds, 28, 166-170.


48. Theelen, R. M. C.; Liem, A. K. D.; Slob, W.; van Wijnen, J. H. (1993). Intake of 2,3,7,8 chlorine substituted dioxins, furans, and planar PCBs from food in the Netherlands: median and distribution, Chemosphere, 27, 1625-1635.
49. van der Velde, E. G.; Marsman, J. A.; de Jong, A. P. J. M.; Hoogerbrugge, R.; Liem, A. K. D. (1994). Analysis and occurrence of toxic planar PCBs, PCDDs and PCDFs in milk by use of carbosphere activated carbon, Chemosphere, 28, 693-702.
50. Choi, D.; Hu, S.; Jeong, J.; Won, K.; Song I. (2000). Levels of dioxin-like compounds in Korea food, Organohalogen Compounds, 47, 375-377.
51. Jeong, G. H.; You, J. C.; Joo, C. H.; Jeon, S. E. (2001). Distribution characteristics of 2,3,7,8-substituted dioxins in the fresh water fishes from the major rivers in S. Korea, Organohalogen Compounds, 51, 247-250.
52. Abad, E.; Llerena, J. J.; Caixach, J.; Rivera, J. (2000). Polychlorinated dibenzo-p-dioxins, dibenzofurans and co-planar biphenyls in foodstuffs samples from Catalonia (Spain), Organohalogen Compounds, 47, 306-309.
53. Jimènez, B.; Hernàndez, L. M.; Eljarrat, E.; Rivera, J.; Gonzàlez, M. J. (1996). Estimated intake of PCDDs, PCDFs and co-planar PCBs in individuals from Madrid (Spain) eating an average diet, Chemosphere, 33, 1465-1474.
54. Focant, J. F.; Massart, A. C.; Eppe, G.; Pirard, C.; André, J. E.; Xhrouet, C.; Pauw, E. D. (2001). Levels and trends of PCDD/Fs and cPCBs in Belgian foodstuffs one year after the “dioxin crisis”, Organohalogen Compounds, 51, 243-246.
55. Amirova, Z.; Kruglov, E.; Donnic, I.; Grosheva, E. (2001). Control instrumentation of PCDD/Fs content in foodstuff in Russia, Organohalogen Compounds, 51, 298-301.
56. Scortichini, G.; Diletti, G.; Torreti, L.; Forti, A. F.; Scarpone, R.; Migliorati, G. (2001). Food and animal feeds contamination by PCDDs-PCDFs in Italy in years 1999 and 2000: incidence and TEQ congeners patterns, Organohalogen Compounds, 51, 400-403.
57. Peng, J. H.; Weng, Y. M. (2001). PCDDs, PCDFs and dioxin-like PCBs in fish from Tung Kang, Kao Ping rivers in Taiwan, Organohalogen Compounds, 51, 364-367.
58. 經濟部標準檢驗局:中國國家標準CNS 14758「食品中戴奧辛及多氯聯苯殘留量檢驗方法」。經濟部標準檢驗局,2003年7月。
59. US EPA Method 1668A (1997). Toxic Polychlorinated Biphenyls by Isotope Dilution High Resolution Gas Chromatography / High Resolution Mass Spectrometry, US EPA.
60. Malisch, R.; Baumann, B.; Behnisch, P. A.; Canady, R.; Fraisse, D.; Fürst, P.; Hayward, D.; Hoogenboom, R.; Hoogerbrugge, R.; Liem, D.; Päpke, O.; Traag, W.; Wiesmüller, T. (2001). Harmonised quality criteria for chemical and bioassays analyses of PCDDs/PCDFs in feed and food -- Part 1: general considerations, GC/MS methods Organohalogen Compounds, 50, 53-58.
61. Global Environment Monitoring System/Food Contamination Monitoring and Assessment Programme (GEMS/Food) (2003). GEMS/Food Regional Diets -- Regional per Capita Consumption Of Raw and Semi-processed Agricultural Commodities, GEMS/Food, WHO.

Chapter 3
1. 台灣地區食品營養成分資料庫 (1998),行政院衛生署。
2. 台灣地區食品營養成分資料庫(二) (2002),行政院衛生署。
3. 常見食品營養圖鑑 (1998),行政院衛生署。
4. 民國89年漁業年報,行政院農業委員會漁業署http://www.fa.gov.tw/tfb7/2000c.htm
5. 91年度農業統計年報,行政院農業委員會 http://agr.pdaf.gov.tw/list.htm
6. 內政統計月報 (93年5月),行政院內政部http://www.moi.gov.tw/stat/month/m1-01.xls
7. Joint FAO/WHO Expert Committee on Food Additives (JECFA) (2001). Summary and conclusions of the fifty-seventh meeting, JECFA.
8. 農業統計月報,農產加工業主要產品產銷存量值 (93年5月) 行政院農業委員會。 http://www.coa.gov.tw/statistic/mon/t33.htm
9. 鄭速珍 (1999),我國乳製品產業供需現況分析,食品市場資訊,8803期。
10. 許可嬰兒配方奶粉相關資訊,食品衛生處,行政院衛生署http://www.doh.gov.tw/org2/b3/1212-1.htm
11. 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.; Zacharewski, T. (1998). Toxic Equivalency Factors (TEFs) for PCBs, PCDDs, PCDFs for humans and wildlife, Environmental Health Perspectives, 106, 775-792.
12. World Health Organization (1998). Executive Summary: Assessment of the health risk of dioxins: re-evaluation of the Tolerable Daily Intake (TDI), WHO Consultation, WHO.
13. Council Regulation No 2375/2001 (2001). Amending Commission Regulation (EC) No 466/2001 setting maximum levels for certain contaminants in foodstuffs, EC.
14. Malisch, R. (1998). Update of PCDD/PCDF-intake from food in Germany, Chemosphere, 37, 1687-1698.
15. Schuler, F.; Schmid, P.; Schlatter, Ch. (1997). The transfer of polychlorinated dibenzo-p-dioxins and dibenzofurans from soil into eggs of foraging chicken, Chemosphere, 34, 711-718.
16. European Commission (2000). Reports on tasks for scientific cooperation (SCOOP). Assessment of dietary intake of dioxins and related PCBs by the population of EU Member States, Report of experts participating in Task 3.2.5, 7, Directorate-General Health and Consumer Protection, EC.
17. European POPs Expert Team, EPET (2002). Preparatory actions in the field of dioxin and PCBs – Executive Summary, EC.
18. 經濟部標準檢驗局:中國國家標準CNS 5036「食品中粗脂肪之檢驗方法」。經濟部標準檢驗局,1984年1月。
19. 經濟部標準檢驗局:中國國家標準CNS 3444「乳品檢驗法--乳脂肪之測定」。經濟部標準檢驗局,1996年9月。
20. US EPA Method 1613B (1994). Tetra- through Octa-Chlorinated Dioxins and Furans by Isotope Dilution HRGC/HRMS, US EPA.

Chapter 4
1. Wu, S. J.; Chang, Y. H.; Fang, C. W.; Pan, W. H. (1999). Food sources of weight, calories, and three macro-nutrients-NAHSIT 1993-1996, Nutritional Sciences Journal, 24, 41-58.
2. 91年度農業統計年報,行政院農業委員會 http://agr.pdaf.gov.tw/list.htm
3. 農業統計月報,農產加工業主要產品產銷存量值 (93年5月) 行政院農業委員會。
http://www.coa.gov.tw/statistic/mon/t33.htm
4. 民國91年漁業年報,行政院農業委員會漁業署http://www.fa.gov.tw/tfb7/2002c.htm
5. 台灣地區食品營養成分資料庫 (1998),行政院衛生署。
6. 台灣地區食品營養成分資料庫(二) (2002),行政院衛生署。

Chapter 5
1. Chlorine Chemistry Council (CCC) (2002). A comparison of dioxin risk characterizations, American Chemistry Council.
2. World Health Organization (1998). Executive Summary: Assessment of the health risk of dioxins: re-evaluation of the Tolerable Daily Intake (TDI), WHO Consultation, WHO.
3. Joint FAO/WHO Expert Committee on Food Additives (JECFA) (2001). Summary and conclusions of the fifty-seventh meeting, JECFA.
4. Scientific Committee on Food (SCF) (2000). Opinion of the SCF on the risk assessment of dioxins and dioxin-like PCBs in food, SCF/CS/CNTM/DIOXIN/8 FINAL, SCF, EC.
5. Committee on Toxicity of Chemicals in Food, Consumer Products and the Environment (COT) (2001). Statement on the tolerable daily intake for dioxins and dioxin-like polychlorinated biphenyls, Department of Health, UK.
6. Environmental Health Committee of the Central Environment Council (Environment Agency) and Living Environment Council and Food Sanitation Investigation Council (Ministry of Health and Welfare) (1999). Report on Tolerable Daily Intake (TDI) of dioxins and related compounds, Ministry of Health and Welfare, Japan.
7. Hsu, M. S.; Ma, E.; Cheng, P. S.; Chou, U.; Chen, S. Y.; Chang, C. F.; Chou, S. S.; Cheng, C. C.; Yu, C. Y.; Liao, C. H.; Ling, Y. C. (2002). Levels of PCDD/DFs in foodstuffs in Taiwan, Organohalogen Compounds, 57, 73-76.
8. Malisch, R. (1998). Update of PCDD/PCDF-Intake from food in Germany, Chemosphere, 37, 1687-1698.
9. Food Standards Agency (FSA) (2003). Dioxins and Dioxin-like PCBs in the UK diet: 2001 Total Diet Study samples, Food Surveillance Information Sheet 38/03, FSA, UK.
10. Focant, J. F.; Eppe, G.; Pirard, C.; Massart, A. C.; André, J. E.; Pauw, E. De (2002). Levels and congener distributions of PCDDs, PCDFs and non-ortho PCBs in Belgian foodstuffs: Assessment of dietary intake, Chemosphere, 48, 167-179.

11. Food and Environmental Hygiene Department (2002). Dietary exposure to dioxins of secondary school students, Food and Environmental Hygiene Department, HKSAR.

12. Wu, Y.; Li, J.; Zhao, Y.; Chen, Z.; Li, W.; Chen, J. (2002). Dietary intake of ploychloranited dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) in populations from China, Organohalogen Compounds, 57, 221-223.
13. Tsutsumi, T.; Yanagi, T.; Nakamura, M.; Kono, Y.; Uchibe, H.; Iida, T.; Hori, T.; Nakagawa, R.; Tobiishi, K.; Matsuda, R.; Sasaki, K.; Toyoda, M. (2001). Update of daily intake of PCDDs, PCDFs, and dioxin-like PCBs from food in Japan, Chemoshpere, 45, 1129-1137.
14. Schecter, A.; Cramer, P.; Boggess, K.; Stanley, J.; Päpke, O.; Olson, J.; Silver, A.; Schmitz, M. (2001). Intake of dioxins and related compounds from food in the U.S. population, Journal of Toxicology and Environmental Health Part A, 63, 1-18.
15. Jimènez, B.; Hernàndez, L. M.; Eljarrat, E.; Rivera, J.; Gonzàlez, M. J. (1996). Estimated intake of PCDDs, PCDFs and co-planar PCBs in individuals from Madrid (Spain) eating an average diet, Chemosphere, 33, 1465-1474.
16. Global Environment Monitoring System/Food Contamination Monitoring and Assessment Programme (GEMS/Food) (2003). GEMS/Food Regional Diets -- Regional per Capita Consumption Of Raw and Semi-processed Agricultural Commodities, GEMS/Food, WHO.
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