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题名: 我国地表水中多类别 PPCPs和农药分析方法的建立及其分布特征研究
作者: 许美佳1
学位类别: 硕士
答辩日期: 2017-05
授予单位: 中国科学院大学
授予地点: 北京
导师: 王东红 ; 罗茜
关键词: 药物和个人护理品(PPCPs),农药,地表水,水库型地表水,污水 ; pharmaceuticals and personal care products (PPCPs), pesticides, surfacewater, reservoir water, sewage
其他题名: Establishment of analytical method and distribution of multi-class PPCPs and pesticides in surface water in China
学位专业: 环境科学
中文摘要: 药物和个人护理品(pharmaceuticals and personal care products, PPCPs)及 农药是水中普遍存在的 2大类有机污染物,其具有种类繁多、理化性质差异大 且在水中浓度水平低(ng/L或 μg/L)等特点,因此,同时分析水中多类别 PPCPs 和农药面临着一定的困难。本论文在实验室原有方法的基础上进行了前处理方 法和仪器分析方法的优化,最终建立了一种基于固相萃取法( SPE)和超高效 液相色谱串联质谱联用仪(UPLC-MS/MS)用于同时提取和快速检测水中 130 种 PPCPs和 35种农药的分析方法。该方法线性良好且灵敏度和回收率较高, 可较快速准确检测水中痕量的 PPCPs和农药。本论文将所构建的分析方法应用 于我国地表水和污水中 PPCPs和农药污染分布特征的研究,包括了我国重点流 域地表水、珠江流域水库型地表水以及北京市地表水和污水处理厂出厂水。 在我国 7个重点流域地表水中,共检出 122种目标化合物(103种 PPCPs 和 19种农药),其平均检出浓度范围为 0.02~332.75 ng/L。抗生素类药物是最主 要检出的 PPCPs类污染物,其中又以磺胺类和喹诺酮类为主;检出的非抗生素 类 PPCPs主要是皮质激素、雄激素、孕激素和雌激素,但其检出率和检出浓度 均普遍偏低;避蚊胺是最主要检出的个人护理品,在所有地表水采样点中均被 检出(检出率为 100%);农药污染物主要为有机磷类农药和氨基甲酸酯类农药。 东江流域是本次调查中 PPCPs和农药污染最严重的流域,其检出的 PPCPs和农 药污染物种数最多(87种)且这些污染物的检出平均浓度总和最高(3713 ng/L)。 珠江流域水库型地表水中 PPCPs和农药的调查结果表明仅 69种目标化合 物(49种 PPCPs和 20种农药)被检出,其在冬夏 2个季节中的检出浓度范围 均典型为几 ng/L至几十 ng/L。珠江流域水库型地表水中最主要检出的 PPCPs 类别也为抗生素类药物且也以磺胺类和喹诺酮类为主,而有机磷类农药和氨基 甲酸酯类农药也是最主要检出的农药类别。大部分目标化合物在夏季的检出浓 度比冬季低,可能是受 PPCPs和农药季节性排放量、水体径流量稀释效应、水 体温度和光照强度等因素的影响。在不同城市水库型地表水中目标化合物的存 在情况则主要受到地理位置、周围环境、人口密度和季节变化等因素的影响。 北京市 5大水系地表水和 8个行政区/县污水处理厂出厂水中分别检出了 151种(118种 PPCPs和 33种农药)和 138种(110种 PPCPs和 28种农药)目 标化合物,且检出的目标化合物类别是一致的。绝大多数目标化合物的检出浓 度均在 1000 ng/L以下,在地表水中有 3种化合物的最大检出浓度超过 1000 ng/L,即脱水红霉素(2151.87 ng/L)、可铁宁(1060.78 ng/L)和避蚊胺(1285.02 ng/L),而在污水处理厂出厂水中只有氧氟沙星(1260.06 ng/L)的最大检出浓 度超过 1000 ng/L。这些高检出浓度的目标化合物应引起足够的重视。
英文摘要: Pharmaceuticals and personal care product (PPCPs) as well as pesticides are two main categories of organic pollutants which are widespread in water. PPCPs and pesticides can be divided into many categories with a wide range of physico-chemical properties and their concentions in water are usually at lower levels (ng/L or μg/L). Therefore, there are some difficulties and challenges in the simulataneous detection and analysis of multi-class PPCPs and pesticides in water. On the basis of the original method of the laboratory, the pretreatment method and the instrument analysis method were optimized. Eventually, an analytical method based on solid phase extraction (SPE) and ultra performance liquid chromatography tandem mass spectrometry (UPLC-MS/MS) was established for simultaneously extracting and rapidly detecting 130 PPCPs and 35 pesticides in water. This analytical method had good linearity as well as high senditivity and recovery, which was sutiable to quickly and accurately detect the trace amount of PPCPs and pesticides in water. In this thesis, the constructed analytical method was applied to study occurrence and distribution of PPCPs and pesticides in surface water and sewage in China, including surface water of major watersheds, reservior surface water of the Pearl River Basin, as well as surface water and effluents of wastewater treatment plants (WWTPs) in Beijing. In surface water of 7 major watersheds in China, a total of 122 target compounds (103 PPCPs and 19 pesticides) were detected and the average detection concentration range was 0.02-332.75 ng/L. Antibiotic were the main category of PPCPs detected in surface water, which mainly included sulfonamides and quinolones. Non-antibiotic pharmaceuticals detected in surface water mainly included corticosteroids, androgens, progesterones and estrogens, but the detection frequencies and concentrations of most non-antibiotic pharmaceuticals were genelally low. Diethyltoluamide (DEET) was the most frequently detected personal care products, which was found in all sampling sites in surface water (detection frequency=100%). Pesticides contaminants were mainly organophosphorus and carbamate pesticides. In this study, the pollution of PPCPs and pesticides in Dongjiang watershed was the most serious. In Dongjiang watershed, the total number of detected PPCPs and pesticides contaminants was the highest (87 compounds) and the sum of the average concentrations of PPCPs and pesticides was highest (3713 ng/L). The results of PPCPs and pesticides in reservoir surface water of the Pearl River Basin showed only 69 target compouds (49 PPCPs and 20 pesticides) were detected, and their concentrations range in both winter and summer were typically from several ng/L to tens of ng/L. In reservoir surface water of the Pearl River Basin, the most frequently detected category of PPCPs were also antibiotics, and the two main antibiotic categories were still sulfamides and quinolones. Similary, organophosphorus and carbamate pesticides were also the most frequently detected pesticides categories in reservoir surface water of the Pearl River Basin. The concentrations of most target compounds detected in summer were lower than those detected in winter, which could be influenced by the season emissions of PPCPs and pesticides, dilution effect of the water runoff, water temperature and light intensity. Occurrence of target compounds in reservoir surface water in different cities mainly affected by geographical location, surrounding environment, population density and seasonal variation. The occurrences and concentrations of PPCPs and pesticides in surface water from 5 major river systems and effluents of WWTPs from 8 administrative districts in Beijing were investigated. 151 target compouds (118 PPCPs and 33 pesticides) and 138 target compouds (110 PPCPs and 28 pesticides) were respectively detected in surface water and effluents of WWTPs in Beijing, and the categories of PPCPs and pesticides detected in both surface water and effluents of WWTPs were the same. For most of the target compounds, their detection concentrations were below 1000 ng/L. However, there were 3 compounds whose maximum detection concentrations exceeded 1000 ng/L in surface water, namely, erythromycin anhydrate (2151.87 ng/L), cotinne (1060.78 ng/L) and DEET (1285.02 ng/L). For the the effluents of WWTPs, ofloxacin (1260.06 ng/L) was the only compound whose maximum detection concentrations was larger than 1000 ng/L. Therefore, these target compounds with high concentrations in both surface water and effluents of WWTPs should be given sufficient attention.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38723
Appears in Collections:环境化学与生态毒理学国家重点实验室_学位论文

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作者单位: 1.中国科学院生态环境研究中心

Recommended Citation:
许美佳. 我国地表水中多类别 PPCPs和农药分析方法的建立及其分布特征研究[D]. 北京. 中国科学院大学. 2017.
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