| 题名 | 再生水灌溉典型药物土壤环境行为与生态风险研究 |
| 作者 | 伊丽丽 |
| 学位类别 | 博士 |
| 答辩日期 | 2013-05 |
| 授予单位 | 中国科学院研究生院 |
| 授予地点 | 北京 |
| 导师 | 陈卫平 |
| 关键词 | 药物 再生水利用 土壤环境行为 HYDRUS-1D模型 生态风险 pharmaceuticals utilization of reclaimed water environment behaviors in soil HYDRUS-1D model ecological risk |
| 其他题名 | Study on the Environmental Behaviors and Its Potential Ecological Risk of Typical Pharmaceuticals in Soil Receiving Reclaimed Water Irrigation |
| 学位专业 | 生态学 |
| 中文摘要 | 近年来，我国再生水利用事业发展迅速，大量再生水被用于灌溉，然而对于再生水灌溉利用的潜在生态风险认识不足，特别是与药物相关的生态风险。药物是再生水中存在的一大类新型痕量有机污染物，其生态风险已引起相关学者和管理部门的重视。本研究以揭示城市再生水灌溉下典型药物的土壤环境行为及生态风险为总体目标，开展了以下工作： 建立了再生水及土壤中典型药物的同步分析方法。采用固相萃取（SPE）结合超高效液相色谱串联质谱（UPLC-MS/MS）技术，建立了再生水及土壤中8 种药物（氧氟沙星、环丙沙星、诺氟沙星、磺胺嘧啶、磺胺甲恶唑、四环素、土霉素、布洛芬）同步检测的分析方法。研究结果表明：通过优化色谱和质谱参数，8 种药物可以在13 min内实现较好的分离。添加浓度为500 μg·L-1、100 μg·L-1时，水样中药物的回收率为60.1～87.8%，相对标准偏差均小于14.2%；添加浓度为500 μg·kg-1、100 μg·kg-1时，土壤中药物的回收率为51.1～87.3%，相对标准偏差均小于20.2%。以3倍信噪比计算出8 种药物在水、土壤中的检出限分别为：0.98～24.82 ng·L-1、1.53～36.77 μg·kg-1。 吸附是影响污染物在土壤环境中迁移转化的重要过程之一。为揭示典型药物在土壤中的吸附特征，以7 种药物（氧氟沙星、环丙沙星、诺氟沙星、磺胺嘧啶、磺胺甲恶唑、四环素、土霉素）作为研究对象，采用静态吸附试验研究其在北京市潮土土壤表层（0～20 cm）中的吸附动力学行为和土壤剖面（0～20、20～40、40～60、60～80、80～100 cm）中的吸附热力学行为及其受到土壤环境特征的影响。研究结果表明：7 种药物（氧氟沙星、诺氟沙星、环丙沙星、磺胺嘧啶、磺胺甲恶唑、四环素、土霉素）在土壤中的吸附，呈现先快后慢的反应过程，均可以在24 h内趋于平衡；Elovich方程能很好的描述其在土壤中的吸附动力学过程。不同种类药物在同一深度土层中的吸附系数（Kd）各不相同，吸附强弱顺序为：四环素类抗生素（503.1～5742 L·kg-1）>氟喹诺酮类抗生素（160.7～786.1 L·kg-1）>磺胺类抗生素（3.173～7.893 L·kg-1）。同种药物在不同深度土层的Kd值也存在较大差异，其中四环素类相差2.5倍、氟喹诺酮类相差2.7～3.6倍、磺胺类相差1.1倍。药物自身性质的差异是影响其在土壤中吸附行为的主要因素。剖面土壤理化性质的差异也会对药物在土壤中的吸附行为造成一定影响，土壤阳离子交换量和有机质是其主要的影响因子。降解也是影响污染物在土壤环境中迁移转化的重要过程之一。采用室内培养的方法研究了7种药物（氧氟沙星、环丙沙星、诺氟沙星、磺胺甲恶唑、四环素、土霉素、布洛芬）在北京市潮土土壤剖面（0～20、20～40 、40～60 、60～80、80～100 cm）中的降解动力学以及土壤微生物和剖面土壤性质对7种药物在土壤中降解的影响。研究结果表明：7种药物的降解过程符合一级动力学方程。四环素在剖面土壤中易降解（半衰期t1/2<30 天）；环丙沙星、诺氟沙星、土霉素较易降解（30 天 |
| 英文摘要 | In recent years, utilization of reclaimed water has developed rapidly. A large number of recycled water is used for irrigation. So far, knowledge on the potential ecological risks of recycled water for irrigation use is limited, especially risks associated with pharmaceuticals, which is one type of new trace organic pollutants present in reclaimed water and their ecological risk has attracted great attentions of scholars and managers. In this study, soil environmental behaviors of typical pharmaceuticals and their ecological risk under long-term urban recycled water irrigation were studied. The main results are summarized as follows: An analytical method was developed for the simultaneous determination of 8 kinds of typical pharmaceuticals (Ofloxacin, Ciprofloxacin, Norfloxacin, Sulfadiazine, Sulfamethoxazole, Tetracycline, Oxytetracycline, Ibuprofen) in reclaimed water and soil by solid phase extraction (SPE) combined with ultra performance liquid chromatography-tandem mass spectrometry. The results showed 8 kinds of pharmaceuticals achieved better separation within 13 min by optimizing the parameters of chromatography and mass spectrometry. When spiked at 500 μg·L-1 and 100 μg·L-1, the range of recoveries (in percent) for the target compounds in the reclaimed water were 60.1-87.8% and the relative standard deviations were less than 14.2%. When spiked at 500 μg·kg-1 and 100 μg·kg-1, the range of recoveries for the target compounds in the soil were 51.1-87.3% and the relative standard deviations were less than 20.2%. The limits of quantification (LOQs, S /N = 3) in water and soil were 0.98-24.82 ng·L-1 and 1.53-36.77 μg·kg-1 for 8 kinds of pharmaceuticals, respectively. Adsorption is one of the important processes governing the migration and transformation of pollutants in the soil environment. Based on static adsorption experiments, adsorption kinetic in surface Chao soil profile (0-20 cm) and thermodynamic in Chao soil profiles (0-20, 20-40, 40-60, 60-80, 80-100 cm) of 7 kinds of pharmaceuticals (Ofloxacin, Ciprofloxacin, Norfloxacin, Sulfadiazine, Sulfamethoxazole, Tetracycline, Oxytetracycline)were conducted to reveal the adsorption characteristics of different pharmaceuticals in Chao soil profiles in Beijing. Results showed that 7 kinds of pharmaceuticals could reach to adsorption equilibrium within 24 h with an initial rapid adsorption followed by a slow inner diffusion processes. Elovich equations could fit well with their reaction kinetics. Adsorption coefficient Kd values of different pharmaceuticals in the same soil layer were different, and followed a decreasing order of tetracycline antibiotics (503.1-5742 L·kg-1)>fluoroquinolone antibiotics (160.7-786.1 L·kg-1)>sulfonamide antibiotics (3.173-7.893 L·kg-1). Adsorption coefficient Kd values of the same antibiotic in different soil layers were also different by 2.5 times, 2.7-3.6 times and 1.1 times for tetracyclines, fluoroquinolones and sulfonamides, respectively. Adsorption behaviors of pharmaceuticals in the soil environment were mainly influenced by the properties of pharmaceuticals. Soil physicochemical properties could have also influenced adsorption behaviors of pharmaceuticals, cation exchange capacity and organic matter of soil were main factors. Degradation is also one of the important processes governing the migration and transformation of pollutants in the soil environment. Based on indoor incubation experiments, degradation dynamics of 7 kinds of pharmaceuticals (Ofloxacin, Ciprofloxacin, Norfloxacin, Sulfamethoxazole, Tetracycline, Oxytetracycline, Ibuprofen) in Chao soil profiles (0-20, 20-40, 40-60, 60-80, 80-100 cm) in Beijing were studied. The effects of soil microorganisms and soil properties on the degradation of 7 kinds of pharmaceuticals in Chao soil profiles were also conducted. Results showed that degradation process of 7 kinds of pharmaceuticals in soil profiles could be well matched with the first-order kinetics equation. Tetracycline was easily degradable(half-life t1/2<30 days), Ciprofloxacin, Norfloxacin and Oxytetracycline were more difficultly degradable(30 days |
| 公开日期 | 2014-10-20 |
| 内容类型 | 学位论文 |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/7697]  |
| 专题 | 生态环境研究中心_城市与区域生态国家重点实验室 |
| 推荐引用方式 GB/T 7714 | 伊丽丽. 再生水灌溉典型药物土壤环境行为与生态风险研究[D]. 北京. 中国科学院研究生院. 2013. |
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