珠江流域淡水水生生物中典型内分泌干扰污染物的富集研究
发布时间：2018-08-30 17:42
【摘要】：内分泌干扰污染物(EDCs)是能够模拟/模拟生物体对内源性激素的分子效应,干扰或阻止激素正常合成、释放、结合、代谢等过程的一些天然和人工合成化合物。EDCs可能导致动物生殖系统异常、性别紊乱、免疫力及生育力降低等。EDCs广泛存在于世界各地的多种环境介质中。然而,关于EDCs的生物富集及其机理的系统研究还很有限。为此,本研究选取10种典型EDCs包括对羟基苯甲酸甲酯(MP)、对羟基苯甲酸乙酯(EP)、对羟基苯甲酸丙酯(PP)、对羟基苯甲酸丁酯(BP),邻苯基苯酚(PHP)、三氯生(TCS)、双酚A(BPA)三氯卡班(TCC)及其脱氯产物二环己基碳二亚胺(DCC)和均二苯脲(NCC)。系统研究珠江水系野生淡水水生生物中这些EDCs的富集、生物食物链放大潜力以及相应的影响因素,主要结论如下:(1)采用旋涡振荡-超声波辅助萃取结合凝胶渗透色谱除去大分子有机物干扰,再经硅胶柱层析进一步净化,建立生物样品中微/痕量内分泌干扰污染物的UHPLC-MS/MS分析方法,该方法的定量限为0.1~9.7 ng/g dw,回收率为65.2%~118.0%。(2)除NCC以外,EDCs广泛分布于珠江水系淡水野生生物中。EDCs的分布存在一定的种间差异,TCC只在甲壳纲中检出,且占EDCs总浓度的56%,检出率为100%,次为PHP和MP;而硬骨鱼纲中则以BPA为最,检出率为96.67%,次为TCS和MP。另外,EDCs在生物中的分布与食性呈现出一定的关系,肉食性鱼类脊肉中MP的浓度明显高于其他鱼类,浓度范围为402.52 ng/g lw;肉食性鱼类脊肉中TCS和BPA的浓度明显低于其他鱼类,范围分别为ND和21.90ng/glw。(3)EDCs在珠江水系野生淡水鱼类中的富集水平存在明显的组织差异。MP、TCS和BPA在鱼类组织器官中的浓度和生物富集因子(logBAF)基本上表现为肝脏腩脊肉,说明肝脏的富集能力最强,腩次之,脊肉最弱。(4)EDCs在珠江水系野生淡水鱼类中的分布与其生活环境紧密相关,总的来看,珠江广州河段鱼中EDCs浓度较高,尤其是MP、TCS和BPA;EDCs的生物富集表现出一定的季节特征,如MP、TCS和BPA在广东鲂脊肉中浓度表现为雨季高于旱季。生物的个体特征对其中EDCs的分布存在明显影响,如随生物体重的增加,脊肉中的MP的浓度呈上升趋势,而TCS的浓度呈下降趋势。生物性别也对其中EDCs的富集存在明显影响。如MP在雌性福寿鱼脊肉中的浓度高于雄性,TCS在雌性银鲫鱼和广东鲂脊肉中的浓度亦高于雄性,BPA则在在雌性赤眼鳟和福寿鱼脊肉中的浓度也高于雄性。(5)EDCs有一定的生物放大潜力和子代传递效应。如TCS的营养级放大因子(TMF)为1.62,可能沿生态食物链放大,BPA的TMF为0.92,而MP的TMF为0.33,表明可能随着食物链产生生物稀释作用。MP、TCS和BPA均可能发生母子传递效应。
[Abstract]:Endocrine disrupting pollutant (EDCs) can simulate / simulate the molecular effects of endogenous hormones, interfere with or prevent the normal synthesis, release and binding of hormones. Some natural and synthetic compounds such as metabolism. EDCs may lead to abnormal reproductive system, sex disorder, decreased immunity and fertility, and so on. EDCs are widely found in many environmental media all over the world. However, systematic studies on the bioconcentration and mechanism of EDCs are limited. To that end, In this study, 10 typical EDCs including methyl p-hydroxybenzoate (MP), ethyl p-hydroxybenzoate (EP), propyl p-hydroxybenzoate (PP), p-hydroxybenzoate (BP), p-hydroxybenzoate (PHP), (TCS), bisphenol A (BPA), triclosan (TCC) (TCS),) and their dechlorination were selected. Product dicyclohexyl carbodiimide (DCC) and (NCC). The enrichment of these EDCs in wild freshwater aquatic organisms in the Pearl River system, the amplification potential of biological food chain and the corresponding influencing factors were systematically studied. The main conclusions are as follows: (1) using vortex oscillation-ultrasonic assisted extraction combined with gel permeation chromatography to remove the interference of macromolecular organic matter and further purifying by silica gel column chromatography. A UHPLC-MS/MS method for the determination of micro- / trace endocrine disrupting pollutants in biological samples was established. The quantitative limit of this method is 0.1 ~ 9.7 ng/g dw, recovery rate of 65.2% ~ 118.0. (2) there are some interspecific differences in the distribution of ng/g dw, except NCC in freshwater wildlife of Pearl River system. The detectable rate of the total concentration of EDCs is 56. The detectable rate is 100. The second is PHP and MP;, while BPA is the most. The detection rate is 96.67, the second is TCS and MP., and the second is TCS and MP.. In addition, there was a certain relationship between the distribution of MP and their feeding habits. The concentration of MP in the spinal flesh of carnivorous fish was significantly higher than that of other fishes, and the concentration of TCS and BPA in the spinal flesh of carnivorous fish was significantly lower than that of other fishes in the range of 402.52 ng/g lw;. The range was ND and 21.90 ng / glw. (3) there were significant tissue differences in the enrichment levels of EDCs in wild freshwater fishes in the Pearl River system. The concentrations of EDCs and BPA in fish tissues and organs and bioenrichment factor (logBAF) were basically shown as liver brisket. The results showed that the liver had the strongest enrichment ability, followed by the brisket, and the spinal meat was the weakest. (4) the distribution of EDCs in the wild freshwater fish in the Pearl River system was closely related to its living environment. In general, the concentration of EDCs in the fish in the Guangzhou reach of the Pearl River was higher than that in the fish in the Guangzhou reach of the Pearl River. In particular, the bioconcentration of MP,TCS and BPA;EDCs showed seasonal characteristics, such as the concentration of MP,TCS and BPA in the ridge of Bream bream was higher in rainy season than in dry season. The distribution of EDCs was significantly influenced by the individual characteristics of the organism. For example, with the increase of biological weight, the concentration of MP in spinal meat increased, while the concentration of TCS decreased. Sex also had a significant effect on the enrichment of EDCs. If the concentration of MP in female Fushou fish is higher than that of male in female Carassius auratus and bream, the concentration of MP in female red trout and Fushou fish is also higher than that in male. (5) there is a certain percentage of EDCs in female red trout and Fushou fish. Magnification potential and progeny transfer effect. For example, the nutritional factor (TMF) of TCS is 1.62. the TMF of TCS may be 0.92 along the ecological food chain, while the TMF of MP is 0.33, which indicates that the mother-child transmission effect may occur with the biofilution of food chain.
【学位授予单位】：中国科学院大学(中国科学院广州地球化学研究所)
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X52;X171.5
[Abstract]:Endocrine disrupting pollutant (EDCs) can simulate / simulate the molecular effects of endogenous hormones, interfere with or prevent the normal synthesis, release and binding of hormones. Some natural and synthetic compounds such as metabolism. EDCs may lead to abnormal reproductive system, sex disorder, decreased immunity and fertility, and so on. EDCs are widely found in many environmental media all over the world. However, systematic studies on the bioconcentration and mechanism of EDCs are limited. To that end, In this study, 10 typical EDCs including methyl p-hydroxybenzoate (MP), ethyl p-hydroxybenzoate (EP), propyl p-hydroxybenzoate (PP), p-hydroxybenzoate (BP), p-hydroxybenzoate (PHP), (TCS), bisphenol A (BPA), triclosan (TCC) (TCS),) and their dechlorination were selected. Product dicyclohexyl carbodiimide (DCC) and (NCC). The enrichment of these EDCs in wild freshwater aquatic organisms in the Pearl River system, the amplification potential of biological food chain and the corresponding influencing factors were systematically studied. The main conclusions are as follows: (1) using vortex oscillation-ultrasonic assisted extraction combined with gel permeation chromatography to remove the interference of macromolecular organic matter and further purifying by silica gel column chromatography. A UHPLC-MS/MS method for the determination of micro- / trace endocrine disrupting pollutants in biological samples was established. The quantitative limit of this method is 0.1 ~ 9.7 ng/g dw, recovery rate of 65.2% ~ 118.0. (2) there are some interspecific differences in the distribution of ng/g dw, except NCC in freshwater wildlife of Pearl River system. The detectable rate of the total concentration of EDCs is 56. The detectable rate is 100. The second is PHP and MP;, while BPA is the most. The detection rate is 96.67, the second is TCS and MP., and the second is TCS and MP.. In addition, there was a certain relationship between the distribution of MP and their feeding habits. The concentration of MP in the spinal flesh of carnivorous fish was significantly higher than that of other fishes, and the concentration of TCS and BPA in the spinal flesh of carnivorous fish was significantly lower than that of other fishes in the range of 402.52 ng/g lw;. The range was ND and 21.90 ng / glw. (3) there were significant tissue differences in the enrichment levels of EDCs in wild freshwater fishes in the Pearl River system. The concentrations of EDCs and BPA in fish tissues and organs and bioenrichment factor (logBAF) were basically shown as liver brisket. The results showed that the liver had the strongest enrichment ability, followed by the brisket, and the spinal meat was the weakest. (4) the distribution of EDCs in the wild freshwater fish in the Pearl River system was closely related to its living environment. In general, the concentration of EDCs in the fish in the Guangzhou reach of the Pearl River was higher than that in the fish in the Guangzhou reach of the Pearl River. In particular, the bioconcentration of MP,TCS and BPA;EDCs showed seasonal characteristics, such as the concentration of MP,TCS and BPA in the ridge of Bream bream was higher in rainy season than in dry season. The distribution of EDCs was significantly influenced by the individual characteristics of the organism. For example, with the increase of biological weight, the concentration of MP in spinal meat increased, while the concentration of TCS decreased. Sex also had a significant effect on the enrichment of EDCs. If the concentration of MP in female Fushou fish is higher than that of male in female Carassius auratus and bream, the concentration of MP in female red trout and Fushou fish is also higher than that in male. (5) there is a certain percentage of EDCs in female red trout and Fushou fish. Magnification potential and progeny transfer effect. For example, the nutritional factor (TMF) of TCS is 1.62. the TMF of TCS may be 0.92 along the ecological food chain, while the TMF of MP is 0.33, which indicates that the mother-child transmission effect may occur with the biofilution of food chain.
【学位授予单位】：中国科学院大学(中国科学院广州地球化学研究所)
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X52;X171.5
【参考文献】
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