典型地区溴代阻燃剂人体暴露状况初步研究
摘要
溴代阻燃剂具有良好的阻燃效果,广泛应用于塑料、电子、建筑、纺织等产品与材料中。近年来随着五溴联苯醚(PentaBDE)和八溴联苯醚(OctaBDE)被逐渐禁用和停止生产,十溴联苯醚(DecaBDE)和六溴环十二烷(HBCD)的产量逐渐增加,也导致了其在环境和生物样本中的水平增加。溴代阻燃剂及其代谢产物均对人体存在潜在的健康危害。本研究对溴代阻燃剂生产源典型地区(山东潍坊滨海经济开发区)普通人群血清中的多溴联苯醚(PBDEs)及其羟基代谢产物以及母乳中的PBDEs进行研究,并建立超高效液相色谱-电喷雾离子源-串联三重四极杆质谱(UPLC-ESI-MS-MS)分析人血样品中羟基多溴联苯醚(HO-PBDEs)的方法；研究对经济发达典型地区上海市配对母血、脐带血、母乳中的PBDEs以及母乳中的HBCD水平进行了分析。结果如下：生产源区血清中(n=43)总PBDEs (∑PBDEs)浓度范围为132.7-4563.2 ng/g脂肪,中位数397.3 ng/g脂肪,BDE-209中位数为198.1 ng/g脂肪。HO-PBDEs只在个别血清样品中检出,其中3-HO-BDE-47浓度范围为 上海母血中(n=48)的∑PBDEs为2.2～11543.8 ng/g脂肪,中位数为211.2 ng/g脂肪,BDE-209是含量最高的同族体,中位数为169.7ng/g脂肪,是其他同族体的100倍以上。脐带血中(n=48)∑PBDEs为5.1-3736.9 ng/g脂肪,中位数为162.9 ng/g脂肪；BDE-209中位数为101.1 ng/g脂肪。母乳样本中(n=48)∑PBDEs为17.4～1298.4 ng/g脂肪,中位数50.7 ng/g脂肪。BDE-209中位数40.6 ng/g脂肪,占∑PBDEs的86.5%。新生儿每日经母乳摄入的PBDEs为131.1～9933.3ng/kg体重/天。研究还对48个母乳中HBCD进行了测定,∑HBCD为0.13-37.75 ng/g脂肪,检出率为79%,中位数1.42 ng/g脂肪。a-HBCD为主要的同族体,中位数为1.24 ng/g脂肪,占HBCD,总量的83%。新生儿每日经母乳摄入的HBCD最高可达243.46 ng/kg体重/天。
研究表明,我国生产源区普通人群PBDEs暴露远高于一般水平,从甲状腺异常率来看,PBDEs暴露可能已经给当地居民造成了内分泌方面的健康影响。上海市产妇母血、脐带血和母乳中PBDEs暴露也达到了较高水平,主要表现为BDE-209的暴露,个别值甚至高于生产源区。分析认为这和我国主要生产和使用十溴联苯醚有关。部分脐带血中的PBDEs各同族体浓度高于母血,提示胎儿在母体中就已经有了一定水平暴露。本研究表明新生儿每日经母乳PBDEs和HBCD摄入量对其健康的影响不容忽视,应持续给予关注。
Brominated flame retardant (BFR) are widely used in plastics, electronics, textile and building materials. As the Pentabromodiphenyl ether (PentaBDE) and Octabromodiphenyl ethers (OctaBDE) listing into Stockholm Convention on Persistent Organic Pollutants (POPs), the productions of Decabromodiphenyl ether (DecaBDE) and Hexabromocyclododecane (HBCD) were increased significantly, which lead to their increase concentration in environmental and biological sample. In this study, the PBDEs and hydroxylated PBDEs (HO-PBDEs) in serum and PBDEs in breast milk of general population from Shandong Weifang Binhai Economic Development Zone of BFR production source area were studied. The PBDEs in paired maternal blood, umbilical cord blood, breast milk in Shanghai was studied; meanwhile, the HBCD levels in breast milk was also detected.
The concentration of total PBDEs(SPBDEs) in serum (n=43) from BFR production area ranged from 132.7 to 4563.2 ng/g lipid, with a median 397.3 ng/g lipid, BDE-209 was the most abundant congenner with a median of 198.1 ng/g lipid. Only 3-HO-BDE-47,5-HO-BDE-47, 6-HO-BDE-47 were detected in a few serum sample. The concentration of SPBDEs in breast milk (n=15) ranged from 52.4 to 643.3 ng/g lipid, the median was 125.9 ng/g lipid. In this study,43 serum donors'thyroid abnormal rate up to 33%. Correlation analysis showed that there was a significant positive correlation between PBDEs congers and thyroid hormone. Additionally, the nursing infants'dietary intake of PBDEs via breast milk in production source area was up to 2071.3 ng/kg b.w./day.
The∑PBDEs in maternal blood (n=48) from Shanghai surburb ranged from 2.2 to 11543.8 ng/g lipid (median:211.2 ng/g lipid), BDE-209 was the most abundant congener (median:169.7 ng/g lipid). The correlation between concentration of BDE-209 and the mothers'education level was negative, as well as monthly income. The concentration of∑PBDEs in umbilical cord blood (n=48) was from 5.1 to 3736.9 ng/g lipid (median: 162.9 ng/g lipid); the median of BDE-209 was 101.1 ng/g lipid. The concentration of∑PBDEs in breast milk samples (n=48) were from 17.4 to 1298.4 ng/g lipid (median:50.7 ng/g lipid). BDE-209 was the most abundant congener, accounting for 86.5% of total PBDEs with a median of 40.6 ng/g lipid. The nursing infants'dietary intakes of PBDEs via breast milk were from 131.1 to 9933.3 ng/kg b.w./day. The HBCD detection rate was 79% in Shanghai breast milk, the∑HBCD ranged from 0.13 to 37.75 ng/g lipid, the median was 1.42 ng/g lipid. a-HBCD was the most abundant diastereoisomer and had been detected in 77% samples. The nursing infants' dietary intake of HBCD via breast milk in Shanghai was up to 243.46 ng/kg b.w./day.
The results showed that the PBDEs in general population body in production area was in a higher level. High abnormal thyroid hormone rate among the serum donors indicated PBDEs may had already affected local residents'health. The PBDEs in maternal blood, umbilical cord blood and breast milk in Shanghai reached a very high level, major congner was BDE-209 pollution. The BDE-209 exposure level in human body due to decaBDE as major production in China. Additionally, the nursing infants health risk by the dietary intake of PBDEs and HBCD via breast milk can not be ignored.
研究表明,我国生产源区普通人群PBDEs暴露远高于一般水平,从甲状腺异常率来看,PBDEs暴露可能已经给当地居民造成了内分泌方面的健康影响。上海市产妇母血、脐带血和母乳中PBDEs暴露也达到了较高水平,主要表现为BDE-209的暴露,个别值甚至高于生产源区。分析认为这和我国主要生产和使用十溴联苯醚有关。部分脐带血中的PBDEs各同族体浓度高于母血,提示胎儿在母体中就已经有了一定水平暴露。本研究表明新生儿每日经母乳PBDEs和HBCD摄入量对其健康的影响不容忽视,应持续给予关注。
Brominated flame retardant (BFR) are widely used in plastics, electronics, textile and building materials. As the Pentabromodiphenyl ether (PentaBDE) and Octabromodiphenyl ethers (OctaBDE) listing into Stockholm Convention on Persistent Organic Pollutants (POPs), the productions of Decabromodiphenyl ether (DecaBDE) and Hexabromocyclododecane (HBCD) were increased significantly, which lead to their increase concentration in environmental and biological sample. In this study, the PBDEs and hydroxylated PBDEs (HO-PBDEs) in serum and PBDEs in breast milk of general population from Shandong Weifang Binhai Economic Development Zone of BFR production source area were studied. The PBDEs in paired maternal blood, umbilical cord blood, breast milk in Shanghai was studied; meanwhile, the HBCD levels in breast milk was also detected.
The concentration of total PBDEs(SPBDEs) in serum (n=43) from BFR production area ranged from 132.7 to 4563.2 ng/g lipid, with a median 397.3 ng/g lipid, BDE-209 was the most abundant congenner with a median of 198.1 ng/g lipid. Only 3-HO-BDE-47,5-HO-BDE-47, 6-HO-BDE-47 were detected in a few serum sample. The concentration of SPBDEs in breast milk (n=15) ranged from 52.4 to 643.3 ng/g lipid, the median was 125.9 ng/g lipid. In this study,43 serum donors'thyroid abnormal rate up to 33%. Correlation analysis showed that there was a significant positive correlation between PBDEs congers and thyroid hormone. Additionally, the nursing infants'dietary intake of PBDEs via breast milk in production source area was up to 2071.3 ng/kg b.w./day.
The∑PBDEs in maternal blood (n=48) from Shanghai surburb ranged from 2.2 to 11543.8 ng/g lipid (median:211.2 ng/g lipid), BDE-209 was the most abundant congener (median:169.7 ng/g lipid). The correlation between concentration of BDE-209 and the mothers'education level was negative, as well as monthly income. The concentration of∑PBDEs in umbilical cord blood (n=48) was from 5.1 to 3736.9 ng/g lipid (median: 162.9 ng/g lipid); the median of BDE-209 was 101.1 ng/g lipid. The concentration of∑PBDEs in breast milk samples (n=48) were from 17.4 to 1298.4 ng/g lipid (median:50.7 ng/g lipid). BDE-209 was the most abundant congener, accounting for 86.5% of total PBDEs with a median of 40.6 ng/g lipid. The nursing infants'dietary intakes of PBDEs via breast milk were from 131.1 to 9933.3 ng/kg b.w./day. The HBCD detection rate was 79% in Shanghai breast milk, the∑HBCD ranged from 0.13 to 37.75 ng/g lipid, the median was 1.42 ng/g lipid. a-HBCD was the most abundant diastereoisomer and had been detected in 77% samples. The nursing infants' dietary intake of HBCD via breast milk in Shanghai was up to 243.46 ng/kg b.w./day.
The results showed that the PBDEs in general population body in production area was in a higher level. High abnormal thyroid hormone rate among the serum donors indicated PBDEs may had already affected local residents'health. The PBDEs in maternal blood, umbilical cord blood and breast milk in Shanghai reached a very high level, major congner was BDE-209 pollution. The BDE-209 exposure level in human body due to decaBDE as major production in China. Additionally, the nursing infants health risk by the dietary intake of PBDEs and HBCD via breast milk can not be ignored.
引文
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