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研究生:黃柏菁
研究生(外文):Po-Chin Huang
論文名稱:鄰苯二甲酸酯類環境流布及其對台灣孕婦和新生兒健康影響之相關性研究
論文名稱(外文):Occurrence of Phthalates and Association between Phthalates Exposure and Health Effects of Pregnant Women and Newborns in Taiwan
指導教授:李俊璋李俊璋引用關係郭保麟郭保麟引用關係
指導教授(外文):Ching-Chang LeePao-Lin Kuo
學位類別:博士
校院名稱:國立成功大學
系所名稱:環境醫學研究所
學門:醫藥衛生學門
學類:公共衛生學類
論文種類:學術論文
論文出版年:2008
畢業學年度:96
語文別:英文
論文頁數:145
中文關鍵詞:水質指標孕婦鄰苯二甲酸酯類底泥與生物累積係數鄰苯二甲酸酯類代謝物新生兒肛門-生殖器距離甲狀腺素
外文關鍵詞:thyroid hormoneano-genital distancepregnant womennewbornswater quality index.phthalatesBSAFphthalate metabolites
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台灣號稱為塑膠王國,舉凡民生食、衣、住、行、育、樂都離不開塑膠製品,家庭垃圾更有20%以上是屬於塑膠廢棄物。塑膠製品除了陳年不爛,不易分解,造成環境污染外,塑膠成型時所添加之塑化劑—鄰苯二甲酸酯類(Phthalates,簡稱PAEs),更具有干擾內分泌系統之效應。台灣民眾長期使用塑膠產品,但因缺乏良好之回收系統,塑膠相關產品廢棄後是否造成台灣環境PAEs之污染並未有一系統性及全國性的深入探討。此外,PAEs對動物與人類生殖系統均有毒性,會造成實驗動物生殖毒性及死產率上升、抗甲狀腺素及穿越胎盤之能力,然而對人類易感性族群之影響仍未知,尤其是孕婦及新生兒。因此,本研究將調查台灣主要河川中底泥及魚體中PAEs之濃度分布及累積程度,並進一步針對PAEs污染程度較高之地區,進行孕婦及新生兒PAEs之暴露與健康影響之相關性研究。
2004-2005年間一共自17條主要河川中收集了128個底泥樣本,23個單一魚體樣本,及10個混合魚體樣本,並自環保署水質監測站收集水質指標資料,如溶氧、水溫、化學需氧量等。另外,2005-2006年間共完成83位孕婦懷孕早期、78位孕婦懷孕中期、61位孕婦分娩前尿液、血液和臍帶血樣本,以及65位孕婦羊水樣本之採樣與分析工作,另外亦完成一份孕婦飲食習慣、化妝品及個人衛生用品使用習慣之調查問卷,亦完成65位新生兒出生時健康指標如肛門-生殖器距離及胎齡等資料之收集。尿液、羊水及血清樣本皆使用液相層析串連式質譜儀完成五種鄰苯二甲酸酯類代謝物(Phthalate monoester)之分析,而血清樣本則是進行甲狀腺素和性荷爾蒙之檢測。
結果顯示17條主要河川底泥中PAEs以鄰苯二甲酸(2-乙基己基)酯[di-(2-ethylhexyl) phthalate, DEHP)為最高,平均濃度達4.1 mg/kg乾重(枯水期),且枯水期有高於豐水期(1.2 mg/kg乾重)之現象。四項水質指標(化學需氧量、水溫、氨氮及懸浮固體)可能藉由干擾生物降解之過程影響底泥中DEHP之濃度。單一魚體中DEHP平均濃度以大鱗鯔為最高(61.8 mg/kg乾重),其次為吳郭魚(33.6 mg/kg乾重),而此兩種魚體之生物底泥累積係數(BSAF)也偏高,顯示魚體中DEHP之累積可能與魚種之食性和污染物的物化特性有關。
此外,易感性族群之研究結果顯示,孕婦第二妊娠期的暴露皆以mono-butly phthalate (MBP: 81.8 ng/mL)、monoethyl phthalate (MEP: 27.7 ng/mL)及mono-2-ethylhexyl phthalate (MEHP: 20.6 ng/mL)為主,顯示孕婦主要受到鄰苯二甲酸丁基酯(di-n-butyl phthalate, DBP)、鄰苯二甲酸乙基酯(diethyl phthalate, DEP)及DEHP等三種PAEs之暴露。同時,孕婦體內MBP之暴露量與T4及FT4呈現顯著負相關,以多變項回歸分析法將年齡、BMI及懷孕週期進行校正後,發現MBP和T4、FT4亦呈現顯著負相關,顯示孕婦體內DBP之暴露可能為干擾T4及FT4分泌的因子之一;孕婦第一妊娠期及羊水的暴露則以MBP(中位數濃度:78.4及85.2 ng/mL)、MEHP(24.9及22.8 ng/mL)及MEHP(19.8及ND ng/mL)為主,而僅在尿液和羊水中MBP呈現顯著之中度相關,顯示孕婦尿液中PAEs暴露僅能部分反應胎兒子宮內PAEs之暴露。女嬰的羊水中MBP與新生兒肛門-生殖器距離指標(Ano-genital distance index,AGI)呈現顯著之負相關(R= �{0.32),男嬰方面則無顯著之相關性。進一步以迴歸分析,發現羊水中MBP含量與AGI仍呈現顯著之負相關,顯示胎兒早期MBP之暴露可能對女嬰產生抗雄性化之現象;孕婦分娩時尿液中PAEs代謝物皆以MBP(中位數濃度:114 ng/mL)、MEHP(40.2 ng/mL)及MEP(36.4 ng/mL)為主,而血清與臍帶血中PAEs代謝物則是以MBP(中位數:158及256.0 ng/mL)及MEHP(中位數:21及24.7 ng/mL)為主,顯示DBP及DEHP同時具有穿越人類胎盤之能力。同時,也與新生兒甲狀腺素指標(TSH×T4)呈現顯著負相關,進一步以多變項回歸分析後,仍發現臍帶血中MBP與TSH、T4及TSH×T4呈現顯著負相關,顯示胎兒子宮內DBP之暴露可能會影響新生兒之甲狀腺功能。上述結果之相關機制仍有待進一步研究來釐清其相關性。
由於孕婦PAEs之暴露可能對孕婦甲狀腺荷爾蒙及新生兒之健康產生疑慮,且孕婦在懷孕期間可能不自覺的接觸到許多含PAEs之產品,因此,建議孕婦減少化妝品之使用及減少食用含有PVC成份之微波食品等,皆能減少PAEs之暴露。
Phthalates are developmental and reproductive toxicants for the fetus in pregnant rodents, and the ability of phthalates to penetrate the placenta have been reported. Scientific evidences showed probable thyroid-like function of some phthalates in vitro and in vivo, and phthalates exposure can begin in utero. Because phthalates are ubiquitous in daily life, the potential consequences of human exposure to phthalates have raised concerns in susceptible subjects, such as pregnant women, and infants. Therefore, the body burden and health effects of phthalates are a matter of concerned in countries all over the world, particularly in those that use a great many plastics, such as Taiwan.
The aims of this study are (1) to determine the relationships between phthalate levels in sediment and aquatic factors, and biota-sediment accumulation factor (BSAF) for phthalates; (2) to investigate the association between phthalates exposure, and health effects of pregnant Taiwanese women and newborns.
A total number of 128 sediment samples for two seasons, and 23 single fish and 10 pooled fish samples were collected from seventeen selected principal Taiwan’s rivers during 2004 to 2005. Six phthalates, including di-n-butyl phthalate (DBP), butyl benzyl phthalate (BBzP), di(2-ethylhexyl) phthalate (DEHP), were measured in sediment and biota samples by GC/MS. Water quality parameters including dissolvable oxygen, water temperature, chemical oxygen demand (COD), suspended solids, and ammonia-nitrogen, were obtained from the water quality monitoring network of Taiwan’s EPA from the same week as our sampling period. Besides, after signing a consent form, we collected eighty-three, seventy-eight and sixty-one urine, serum and cord blood samples from pregnant Taiwanese women in the first, second and third trimesters, respectively. Sixty-five amniotic fluid samples and the health of newborns were also collected during 2005-2006. Demographic characteristics of our participants were obtained from an administrated questionnaire in the 2nd trimester. Five phthalates monoesters, including mono butyl phthalate (MBP), mono ethyl phthalate (MEP), and mono ethylhexyl phthalate (MEHP), were measured in urine, amniotic fluid, serum and cord blood samples using HPLC-MS/MS. Serum samples were also analyzed for maternal and fetal thyroid hormones, including thyroid stimulating hormone (TSH), triiodothyronine (T3), thyroxine (T4), and free T4 (FT4).
Mean concentrations (range) of DEHP, BBzP and DBP in sediment at low-flow season were 4.1 (<0.05–46.5), 0.22 (<0.05–3.1) and 0.14 (<0.05–1.3) mg kg-1 dw; those at high-flow season were 1.2 (<0.05–13.1), 0.13 (<0.05–0.27) and 0.09 (<0.05–0.22) mg kg-1 dw, respectively. Trace levels of dimethyl phthalate (DMP), diethyl phthalate (DEP) and di-n-octyl phthalate (DOP) in sediment were found in both seasons. Concentrations of DEHP in sediments were significantly affected by temperature, suspended solids, ammonia-nitrogen, and COD. Highest concentration of DEHP in fish samples were found in Liza subviridis (253.9 mg kg-1 dw) and Oreochromis niloticus niloticus (129.5 mg kg-1 dw). BSAF of DEHP in Liza subviridis (13.8–40.9) and Oreochromis miloticus niloticus (2.4–28.5) were higher than those in other fish species, indicating that the living patterns of fish and physical-chemical properties of phthalates, like log Kow, may influence the bioavailability of phthalates in fish. Our data suggested that DEHP level in river sediments were influenced by water quality parameters due to their effects on the biodegradation processes, and that the DEHP level in fish was affected by fish habitat and physiochemical properties of polluted contaminants.
For pregnant women, MBP, MEP and MEHP, the median levels of which were 81.8, 27.7, and 20.6 ng/mL, respectively, were the predominant substances in the urinary phthalate monoesters from the second trimester. Significantly mild negative correlations were found between T4 and urinary MBP (R = -0.248, p < 0.01), and between FT4 and urinary MBP (R = -0.368, p < 0.05). After adjusting for age, BMI, and gestation, urinary MBP levels showed a negative association with FT4 and T4 . Exposure to DBP might affect thyroid activity in pregnant women, but how DBP affects thyroid function is unclear. Further studies are needed to elucidate the mechanism of action or if other factors related to DBP exposure alter the thyroid function.
For newborns, the median levels of three phthalate monoesters in urine and amniotic fluid were 78.4 and 85.2 ng/mL (MBP); 24.9 and 22.8 ng/mL (MEHP); 19.8 and Not Detected (MEP). We found a significant positive correlation only between creatinine adjusted urinary MBP and amniotic fluid MBP (R2 = 0.156, p < 0.05) in all infants and, only in female infants, a significantly negative correlation between amniotic fluid MBP, AGD (R = -0.31, p < 0.05), and the anogenital index adjusted by birth weight (AGI-W) (R = -0.32, p < 0.05). Although the influence of prenatal DBP exposure on the endocrinology and physiology of the fetus is still a puzzle, our data clearly show that in utero exposure to phthalates in general has anti-androgenic effects on the fetus.
On the other hand, MBP and MEHP, the median levels of which were 256.0 and 24.7 ng/mL, respectively, were the predominant substances in cord blood phthalate monoesters. We found a negative correlation between TSH×T4 and MBP in cord blood (R = -0.23, p < 0.05). After maternal age, gestational age, and MEHP in cord blood had been adjusted for, MBP levels in cord blood showed a negative association with TSH (TSH: = -0.217, p < 0.05), T4 (T4: �� = -1.71, p < 0.05), and TSH×T4 (TSH×T4: = -42.8, p < 0.05) in cord blood. Prenatal phthalate exposure may decrease thyroid hormones in newborns. Because aggregate exposure to phthalates is unavoidable in pregnant women, we suggest that pregnant women reduce their contact with products containing a high level of phthalates, particularly cosmetics, and have thyroid function test in their newborns measured.
中文摘要 I
Abstract III
Contents IX
1.Overview of this study - 1 -
2.Literature Reviews - 8 -
2.1 Physicochemical property - 8 -
2.2 Environmental Fate and levels - 10 -
2.3 Toxicological studies - 16 -
2.4. Epidemiological studies - 24 -
3.Occurrence of Phthalates in Sediment and Biota: Relationship to Aquatic Factors, and the Biota-Sediment Accumulation Factor - 27 -
3.1 Introduction - 27 -
3.2 Materials and Methods - 27 -
3.3 Results and Discussion - 34 -
3.4 Conclusion - 48 -
4.Associations between Urinary Phthalate Monoesters and Thyroid Hormones in Pregnant Women - 49 -
4.1 Introduction - 49 -
4.2 Materials and Methods - 50 -
4.3 Results - 55 -
4.4 Discussion - 65 -
4.5 Conclusions - 68 -
5.Association between prenatal exposure to phthalates and the health of newborns - 69 -
5.1 Introduction - 69 -
5.2 Materials and Methods - 70 -
5.3 Results - 75 -
5.4 Discussion - 87 -
5.5 Conclusion - 91 -
6.In utero exposure to phthalates may alter thyroid hormones in newborns - 92 -
6.1 Introduction - 92 -
6.2 Materials and Methods - 93 -
6.3 Results - 97 -
6.4 Discussion - 110 -
7.Summary of significant findings - 114 -
8.References - 116 -
9.Appendixes - 141 -
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