京杭运河及沿岸区域地表水中药物及个人护理品污染地理分布特征及来源辨析
本文选题:京杭运河 + 湖泊 ; 参考:《中国地质科学院》2017年博士论文
【摘要】:药物及个人护理品(PPCPs)是人们以人身健康和个人护理为目的所使用的物质,或是农牧业者为了维持禽畜健康或促进禽畜生长所使用的物质,包含化合物种类繁多。由于PPCPs与人类活动息息相关,而普遍存在于环境中。因其具有一定的生态毒性及生物累积性,而被广泛研究。本论文选取了 45种不同类型的药物与个人护理品,建立了固相萃取-高效液相色谱-四极杆质谱分析方法,并采集分析了京杭运河及沿岸区域的地表水样品。详细分析了京杭运河及沿岸区域地表水中PPCPs的浓度水平及分布规律。系统地比较了京杭运河及相关湖泊与河流中PPCPs的来源。对比了不同季节运河河水中PPCPs分布特征的异同。利用特定PPCPs化合物作为污染的示踪剂,并将受特定污染源影响的湖泊、河流作为指纹片段与京杭运河比较,进而判断京杭运河中药物及个人护理品的来源。为评估与治理京杭运河PPCPs污染提供理论支持。在所有地表水样品中,共检测42种PPCPs化合物被检出,总浓度范围在41.98~1541.87 ng/L。其中夏季运河河水中检出34种,秋季运河36种,湖泊共检出20种,钱塘江27种,淮河29种,海河23种。红霉素、卡马西平、酮洛芬、壬基酚、避蚊胺及阿特拉津在全部样品中均有检出。京杭运河从南至北PPCPs总浓度从城市到农村呈波动分布,城市PPCPs水平高,农村PPCPs水平低。由于不同季节的平均气温,光照强度及降水量差异明显。季节变化对PPCPs的分布影响较大,秋季地表水中PPCPs总浓度明显高于夏季。夏季运河PPCPs总浓度范围为56.3~1177 ng/L,平均值为267 ng/L;秋季运河PPCPs总浓度范围为83.8~1542 ng/L,平均浓度为342ng/L。夏季气温高、光照强、降水量大是PPCPs浓度较低的主要原因。但由于农业活动具有季节性,阿特拉津的喷洒时间也有明显的季节性,所以秋季农闲时运河水中的阿特拉津的平均浓度小于夏季农忙时。京杭运河相关湖泊水样品中PPCPs浓度水平较低,浓度范围为42.0~158ng/L。其中邵伯湖与高邮湖污染浓度最低,可作为人口密度小,远离集中型畜牧业、工业的背景区。太湖为呈城市型、工业型污染特点,骆马湖呈城市型、养殖业型污染特点,南微山湖呈村镇型、生活污水型污染特点。3条京杭运河相关河流PPCPs分布规律各具特点:钱塘江污染水平最低,浓度范围为72.4~188ng/L,平均值113ng/L,以造纸工业园区为分界线,上游为养殖业型污染、下游为工业型污染。淮河样品以抗生素药物为主要污染物,呈典型畜禽养殖业型污染。天津市海河地表水污染最严重,浓度范围为178~502ng/L,平均值为318ng/L,为城市型、生活污水混合污染源型。钱塘江呈现空间尺度上混合污染源的污染特征,淮河主要呈现点源污染的特征,而海河则是城市内河的污染特征。利用主成分统计分析手段,将各湖泊河流作为特征污染源类型指纹对运河个点来源进行比对分析,发现运河中段大部分以畜禽养殖与生活污水混合型污染源为主,而运河两端大城市样品大部分以工业污染与生活污水型污染源为主,运河沿岸农村的样品则以畜禽养殖污染源为主。研究中还对特征性化合物进行了评估与确证。显影剂碘普罗胺为医疗诊断药物,只存在于医疗废弃物,环境样品中的出现指示着医疗废水对环境的污染,可以将碘普罗胺作为城市医疗废水污染的示踪剂。壬基酚与双酚A在所有样品中均有检出,本底值较高,造纸、服装、塑料化工工业与生活污水都是其污染来源,本研究认为本底污染主要来自生活污水,异常高值则主要来自工业污染。阿特拉津的检出率也为100%,作为农用除草剂,对农业污染源有着较好的指示作用。β-内酰胺类抗生素偶有检出,指示新鲜污染源或垃圾渗滤液的污染。
[Abstract]:Drugs and personal care (PPCPs) is a substance used for the purpose of personal health and personal care, or a variety of substances used by farmers and livestock in order to maintain the health of livestock or to promote the growth of livestock. Because PPCPs is closely related to human activities, it is common in the environment. In this paper, 45 different types of drugs and personal care products were selected, and solid phase extraction high performance liquid chromatography (HPLC) quadrupole mass spectrometry was established, and the surface water samples of the Beijing Hangzhou canal and the coastal area were collected and analyzed. The P of the Beijing Hangzhou canal and the coastal area surface water was analyzed in detail. The concentration level and distribution law of PCPs. The sources of PPCPs in the Beijing Hangzhou canal and related lakes and rivers were compared systematically. The similarities and differences of the distribution characteristics of the PPCPs in the canal river in different seasons were compared. The specific PPCPs compounds were used as tracers for pollution, and the lakes and rivers affected by the specific pollution sources were used as fingerprint fragments with Beijing Hangzhou. River comparison, and then determine the sources of drugs and personal care in the Beijing Hangzhou canal, and provide theoretical support for the assessment and management of the PPCPs pollution in the Beijing Hangzhou canal. In all the surface water samples, 42 kinds of PPCPs compounds were detected, the total concentration range was 41.98 to 1541.87 ng/L., among which 34 were found in the summer canal river, 36 of the autumn canals, and the lakes. 20 kinds, 27 species of Qian Tang River, 29 species in Huaihe and 23 species of Haihe River, erythromycin, C Masi Bing, ketoprofen, nonylphenol, repellent and atrazine are detected in all samples. The total concentration of the Jing Hang canal from south to North PPCPs is fluctuating from the city to the countryside, the city PPCPs is high, and the level of PPCPs in the countryside is low. The average temperature in different seasons is the result of the average temperature in different seasons. The difference of light intensity and precipitation is obvious. The seasonal variation has a great influence on the distribution of PPCPs, and the total concentration of PPCPs in the surface water in autumn is obviously higher than that in summer. The total concentration range of the canal PPCPs is 56.3 ~ 1177 ng/L in summer, and the average value is 267 ng/L; the total concentration range of the canal PPCPs is 83.8 ~ 1542 ng/L in the autumn, and the average concentration is higher in the summer temperature of 342ng/L., light in the autumn. Strong precipitation is the main reason for low concentration of PPCPs, but the spraying time of atrazine is also seasonal because of the seasonal characteristics of agricultural activity. So the average concentration of atrazine in the canal water is less than that in summer. The concentration level of PPCPs in the lake water samples related to the Beijing Hangzhou canal is low. From 42 to 158ng/L., the pollution concentration of Shaobo lake and Gaoyou lake is the lowest, which can be used as a small population density, far from the concentrated animal husbandry, and the industrial background area. Taihu is a city type, the industrial type pollution characteristic, the city type of the Lake City, the aquaculture type pollution characteristic, the southern Weishan Lake in the village type, the sewage type pollution characteristic.3 Beijing Hangzhou canal The distribution law of PPCPs in Guan river has the following characteristics: the Qian Tang river has the lowest pollution level, the concentration range is 72.4 ~ 188ng/L, the average value is 113ng/L, which takes the paper industry park as the dividing line, the upstream is the aquaculture pollution and the downstream is industrial type pollution. The Huaihe sample takes the antibiotic drugs as the main pollution contaminant, and presents the typical livestock and poultry pollution type pollution. Tianjin Haihe River The surface water pollution is the most serious, the concentration range is 178 ~ 502ng/L, the average value is 318ng/L, which is the urban type and the mixed pollution source of the domestic sewage. The Qian Tang River presents the pollution characteristics of the mixed pollution source on the space scale, Huaihe mainly presents the characteristics of the point source pollution, while the Haihe River is the pollution characteristic of the inner river in the city. According to the comparison and analysis of the source of the canal, the main source of the canal was found in the middle of the canal. Most of the large cities in the canal were mainly polluted by industrial pollution and domestic sewage, and the rural samples along the canal were the livestock and poultry. The characteristic compounds were also evaluated and confirmed in the study. The developer was used as a medical diagnostic drug, only in medical waste. The appearance of environmental samples indicated the pollution of medical wastewater to the environment. Iplolamine could be used as a tracer for urban medical wastewater pollution. Nonylphenol and bisphenol A could be used as a tracer. In all the samples, the bottom value is higher, paper making, clothing, plastic industry and domestic sewage are the source of pollution. This study suggests that the base pollution mainly comes from domestic sewage, and the abnormal high value is mainly from industrial pollution. The detection rate of atrazine is also 100%. As a agricultural herbicide, it has a better source of agricultural pollution. Indicative effect. Beta lactam antibiotics were detected occasionally to indicate contamination of fresh pollution sources or landfill leachate.
【学位授予单位】:中国地质科学院
【学位级别】:博士
【学位授予年份】:2017
【分类号】:X52
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