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Fate and transport of an estrogen conjugate 17beta-estradiol-17-sulfate in soil-water systems.

机译:雌激素共轭物17β-雌二醇-17-硫酸盐在土壤-水系统中的命运和运输。

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摘要

The hypothesis of this study was that a sulfate conjugated estrogen, i.e. 17beta-estradiol-17-sulfate (E2-17S), could be a precursor to free estrogens detected in the environment. The objectives of were to investigate the fate and transport processes of E2-17S in various soil-water systems. Radiolabeled E2-17S was synthesized using a series of chemical for the subsequent soil batch experiments. The batch experiment results showed that E2-17S dissipated more quickly from the aqueous phase of the topsoil compared to the subsoil, demonstrating that soil organic carbon played a significant role. The aqueous dissipation of E2-17S was attributed to sorption to the soil surface and transformation to form multiple metabolites. The non-linear sorption isotherms indicated limited sorption of E2-17S, and the concentration-dependent log KOC values were 2.20 and 2.45 for the sterile topsoil and subsoil, respectively. The total radioactive residue measured in the irreversible sites was greater than the reversible sites, demonstrating that irreversible sorption was the predominant sorption process. The observed multiple metabolites suggested that E2-17S underwent complex transformation pathways. For the aqueous phase speciation, mono- and di-hydroxy-E2-17S were consistently detected under all soil conditions, which indicated that hydroxylation was the major transformation process. Also, the hydroxyl metabolites were found at higher concentrations in the topsoil than the subsoil. In the reversibly sorbed phase, free estrogens (i.e. 17beta-estradiol and estrone) were detected at relatively low levels (≤ 2% of applied dose) for all soils, demonstrating that deconjugation/hydrolysis and subsequent oxidation did occur. Furthermore, both hydroxylation and hydrolysis of E2-17S took place under the non-sterile and sterile conditions. Although deconjugation was not a major pathway, E2-17S could be a precursor of free estrogens in the environment. A comprehensive one-site fully kinetic model was applied to simulate the overall governing processes in the soil-water systems and to describe the distribution of multiple metabolites in the aqueous, reversibly sorbed, and irreversibly sorbed phases.. The model gave rise to a satisfactory fit for all experimental data obtained from the batch studies, and the 36 estimated parameters were derived at relatively high confidence.
机译:这项研究的假设是,硫酸盐结合的雌激素,即17β-雌二醇-17-硫酸盐(E2-17S),可能是在环境中检测到的游离雌激素的前体。的目的是调查E2-17S在各种土壤-水系统中的命运和运输过程。使用一系列化学物质合成了放射性标记的E2-17S,用于随后的土壤批处理实验。批处理实验结果表明,与底土相比,E2-17S从表土的水相中消散的速度更快,这表明土壤有机碳发挥了重要作用。 E2-17S的水消散归因于土壤表面的吸附和转化形成多种代谢产物。非线性吸附等温线表明对E2-17S的吸附有限,无菌表层土和下层土的浓度依赖性log KOC值分别为2.20和2.45。在不可逆位点测得的总放射性残留量大于可逆位点,表明不可逆吸附是主要的吸附过程。观察到的多种代谢产物表明E2-17S经历了复杂的转化途径。对于水相形态分析,在所有土壤条件下均检测到单羟基和二羟基E2-17S,这表明羟基化是主要的转化过程。而且,发现表层土壤中的羟基代谢物浓度高于地下土壤。在可逆吸附相中,所有土壤中游离雌激素(即17β-雌二醇和雌酮)的含量都相对较低(≤施用剂量的2%),表明确实发生了脱结合/水解和随后的氧化作用。此外,E2-17S的羟基化和水解均在非无菌和无菌条件下进行。尽管解偶联不是主要途径,但E2-17S可能是环境中游离雌激素的前体。应用一个综合的一站式全动力学模型来模拟土壤-水系统中的总体控制过程,并描述多种代谢物在水相,可逆吸附和不可逆吸附相中的分布。该模型产生了令人满意的结果拟合从批处理研究获得的所有实验数据,并且以相对较高的置信度得出了36个估计参数。

著录项

  • 作者

    Bai, Xuelian.;

  • 作者单位

    North Dakota State University.;

  • 授予单位 North Dakota State University.;
  • 学科 Soil sciences.;Agriculture.;Environmental science.
  • 学位 Ph.D.
  • 年度 2013
  • 页码 182 p.
  • 总页数 182
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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