全国农田土壤内分泌干扰效应的生态风险评价

发布时间：2018-04-04 15:01

  本文选题：内分泌干扰物　切入点：甾体激素受体　出处：《浙江大学》2017年硕士论文

【摘要】：中国的土壤污染呈越来越严重的趋势。我国当前对土壤污染物的甄别和鉴定主要是基于现有的土壤环境质量标准和环境安全值,但是随着工农业高速发展,污染物展现出种类多、来源广的特点,现有的相关规定和标准中关于污染物的基本毒性数据有限甚至缺失、针对污染物的有效且准确的化学检测方法缺乏,因此已渐渐不能满足需要,给现代环境污染的管理和控制带来了困难。以往对土壤污染的研究聚焦于污染物的时空分布,对复合污染引发的生态毒理效应的关注不高。然而环境中污染物造成的生态影响和健康风险往往是长期低剂量暴露的结果,简单的通过测定污染物浓度来评价其危害和影响是不够准确的。因此,有必要采用生物学的方法综合评价土壤污染情况。我们前期的研究表明,中国农田土壤中检出许多典型的环境内分泌干扰物(Endocrine Disrupting Chemicals,EDCs),如有机氯杀虫剂、多氯联苯化合物(PCBs)、多环芳烃化合物(PAHs)以及邻苯二甲酸酯类(PAEs)等。这些EDCs可通过模拟内源性甾体激素与其受体结合,产生类激素活性或抗激素活性。甾体激素受体包括雌激素受体(Estrogen Receptor,ER)、雄激素受体(Androgen Receptor,AR)、孕激素受体(Progesterone Receptor,PR)、糖皮质激素受体(Glucocorticoid Receptor,GR)和盐皮质激素受体(Mineralocorticoid Receptor,MR)。已有大量研究表明,EDCs可与ER、AR作用,然而关于EDCs与PR、GR、MR作用的研究相对较少。土壤环境中还存在很多未知的污染物,生物学的方法评价土壤提取物的内分泌干扰效应,可综合评价包含未知污染物的总体内分泌干扰效应情况,因此更利于了解土壤中EDCs的生态风险。本研究采集了全国31个省或地区共122个农田表层土壤,经索氏法提取土壤中有机污染物,利用双荧光素酶报告基因系统检测了土壤提取物通过ER、AR、PR、GR以及MR介导的类/抗甾体激素活性,阐明了EDCs在我国农田土壤中的分布特征及生态风险情况。本研究结果表明:(1)79%土壤提取物样品具有类雌激素活性,雌二醇当量(EEQ)的范围为0～7.34 ng EEQ kg~(-1) soil(d.w.),平均值为1.94 ng EEQ kg~(-1) soil(d.w.),其中东北、北方以及东南部分地区的土壤样品类雌激素活性较高,然而只有16%的土壤样品有抗雌激素活性,它莫西芬当量(ER拮抗剂,TEQ)的范围为0～1535.71μgTEQ kg~(-1) soil(d.w.),平均值为28.37μg FEQ kg~(-1) soil(d.w.),贵州、山西、西藏等地的土壤样品抗雌激素活性显著较高。(2)30%土壤提取物样品具有类雄激素活性,二氢睾酮当量(DEQ)的范围为0~(-1)05.68 ng DEQ kg~(-1) soil(d.w.),平均值为6.88 ng EEQ kg~(-1) soil(d.w.),山东、浙江、云南等地区的土壤类雄激素活性较高。54%土壤样品表现出抗雄激素活性,氟他胺当量(AR拮抗剂,FEQ)范围为0～410.17μg FEQ kg~(-1) soil(d.w.),平均活性是141.01μg FEQ kg~(-1) soil(d.w.),在中部、东南沿海和西南一些地方的土壤样品具有较高的抗雄激素活性。(3)32%土壤提取物样品具有类孕激素活性,孕酮当量(PEQ)的范围为0-2070.28 ng PEQ kg~(-1) soil(d.w.),平均值为43.10ng PEQ kg~(-1) soil(d.w.),其中福建漳州的土壤提取物表现出非常高的类孕激素活性。73%土壤提取物样品具有抗孕激素活性,米非司酮当量(PR拮抗剂,REQ)范围为0～12.58μg REQ kg~(-1) soil(d.w.),平均抗孕激素活性值为2.65μg REQ kg~(-1) soil(d.w.),除辽宁、天津、新疆外,全国的土壤提取物样品普遍存在抗孕激素活性。(4)35%土壤提取物样品具有类糖皮质激素活性,皮质醇当量(HEQ)范围为0~(-1)48.15 ng HEQ kg~(-1) soil(d.w.),平均值为18.31 ng HEQ kg~(-1) soil(d.w.),上海、江苏、辽宁等地的土壤样品类糖皮质激素效应较显著;59%土壤提取物样品具有抗糖皮质激素活性,米非司酮当量(GR拮抗剂,REQ)范围在0～12.26μg REQ kg~(-1) soil(d.w.)之间,平均抗糖皮质激素活性值为3.23μg REQ kg~(-1) soil(d.w.),南方地区土壤样品的抗糖皮质激素活性较北方高,东部较西部高。(5)72%和78%的土壤提取物样品分别具有类盐皮质激素活性和抗盐皮质激素活性,其中醛固酮当量(AEQ)范围为0～25.64 ng AEQ kg~(-1) soil(d.w.),平均类盐皮质激素活性为1.82 ng AEQ kg~(-1) soil(d.w.),螺内脂当量(MR拮抗剂,SEQ)范围为0～87.7μg SEQ kg~(-1)(d.w.),平均抗盐皮质激素活性值为27.82μg SEQ kg~(-1)(d.w.),全国各地的土壤样品广泛存在类/抗盐皮质激素活性。综上所述,本研究发展了以离体细胞实验的内分泌干扰效应来评价区域生态风险的方法体系,并应用这些方法评估了全国农田土壤EDCs污染的生态风险。
[Abstract]:Soil pollution China is more and more serious trend. China's current screening and identification of soil pollutants mainly existing soil environmental quality standard and environmental safety based on the value, but with the rapid development of industry and agriculture, pollutants show variety, wide source characteristics, the existing relevant provisions and standards of basic pollutants according to the Limited toxicity data or lack of effective and accurate detection method of chemical pollutants lack, therefore has been gradually unable to meet the needs of management and control for the modern environmental pollution is difficult. The previous research on soil pollution pollutants focused on the spatial and temporal distribution of ecotoxicological effects due to the complex pollution concern is not high however. The ecological impact of pollutants in the environment and health risks are often long-term low dose exposure results, simply by measuring the concentration of pollutants. The price of its harm and influence is not accurate. Therefore, it is necessary to adopt the method of comprehensive evaluation of soil biological pollution. Our previous study showed that many typical environmental endocrine disruptors (Endocrine Chinese in detection of soil Disrupting Chemicals, EDCs), such as organochlorine pesticides, polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs) and the adjacent benzene two formic acid ester (PAEs). These EDCs can be combined through the simulation of endogenous steroid hormone receptor, produce hormones or hormone activity. The activity of anti steroid hormone receptors including estrogen receptor (Estrogen, Receptor, ER, androgen receptor (Androgen) Receptor, AR (Progesterone), progesterone receptor Receptor. PR), glucocorticoid receptor (Glucocorticoid, Receptor, GR) and mineralocorticoid receptor (Mineralocorticoid, Receptor, MR). There are a large number of studies show that EDCs and ER, AR However, about EDCs and PR, GR, the function of MR is relatively small. There are still many unknown contaminants in the soil environment, the endocrine disrupting effects of biological evaluation methods of soil extract, comprehensive evaluation contains unknown pollutants the endocrine disrupting effects of the overall situation, and therefore more conducive to understanding the ecological risk of EDCs in soil. Study on the acquisition of the country's 31 provinces or regions of 122 topsoil, the extraction of organic pollutants in soil by Soxhlet method, using dual luciferase reporter assay system was used to extract soil by ER, AR, PR, GR and MR mediated / anti steroid hormone activity, the EDCs distribution characteristics and ecological the risk in China's farmland soil. The results of this study show that: (1) 79% soil extract samples the estrogenic activity, estradiol equivalent (EEQ) in the range of 0 ~ 7.34 ng EEQ kg~ (-1) soil (D.W.), 骞冲潎鍊间负1.94 ng EEQ kg~(-1) soil(d.w.),鍏朵腑涓滃寳,鍖楁柟浠ュ強涓滃崡閮ㄥ垎鍦板尯鐨勫湡澹ゆ牱鍝佺被闆屾縺绱犳椿鎬ц緝楂，

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