大凌河口地区有机氯农药污染特征研究
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摘要
有机氯农药(Organochlorine Pesticides, OCPs)属于典型的持久性有机污染物(Persistent Organic Pollutants, POPs),由于具有毒性、长期残留性、半挥发性和生物富集性,因此严重危害环境及人体健康,已成为目前倍受关注的全球性环境问题。研究OCPs在多介质环境中的分布特征、迁移转化规律及生态毒理是探究其在全球污染水平、分配行为和生态风险的重要组成部分。本研究于2011～2012年,连续采集大凌河口地区多介质环境(土壤、水体、沉积物)样品,利用GC-ECD测定22种OCPs,研究该地区多介质环境中OCPs的残留现状、污染水平、分布特征和污染来源,进而探究影响残留分布的控制因素。本文有利于掌握大凌河口地区OCPs污染的确实情况,为生态环境修复与管理提供理论依据及技术支持,对保障人民生命健康与安全具有现实意义。
本论文第一部分建立了大凌河流域有机氯农药历史使用清单,并在此基础上估算了该地区OCPs排放量与土壤残留量。在统计大量使用数据的基础上,本文利用地理信息系统和Access数据库,建立了我国大凌河流域1/4°经度×1/6°纬度分辨率的网格化的HCHs和DDTs的使用清单,使用清单从空间分布上量化了大凌河流域环境中HCHs和DDTs的来源。从1952～1984年间,大凌河流域HCHs和DDTs的使用量分别为18kt和910t。在使用清单的基础上,以SGPERM模型为工具,估算得出大凌河流域1960～2010年间环境中HCHs和DDTs的排放量为5600t和510t、土壤残留量在2010年分别为2.2t和10.2t。
本论文第二部分对大凌河中下游主要城市(凌海市)城区土壤中有机氯农药污染特征进行研究。结果表明：土壤中22种OCPs均有不同程度的检出,其中HCHs及其异构体和DDTs及其降解产物的检出率及残留量较高。土壤HCHs残留量均符合中国一级土壤标准(GB15618-1995),生态风险较低；部分土壤样品DDTs含量超出中国一级土壤标准,对当地土壤生物和鸟类具有一定的潜在生态风险。采用异构体比值法对土壤中HCHs和DDTs的来源进行初步判定,表明该地区土壤中HCHs和DDTs主要来自于历史上的残留,但近期部分地区有林丹和三氯杀螨醇的使用。表层土壤有机氯农药残留量受不同土地利用方式、上壤有机碳含量、土壤含水量和土壤粘粒含量影响显著(P<0.05)。利用多元地统计和地理信息系统GIS (Geographic Information System)相结合的分析方法,对凌海地区OCPs的空间分布进行研究表明,不同种类OCPs在研究区分布存在很大差异。
本论文第三部分对大凌河口地区水体中有机氯农药污染特征进行研究。结果显示：表层水体22种OCPs含量均有不同程度的检出,其中检出率和残留量较高的组分是HCHs和DDTS。经健康风险评价,该地区水体中HCHs和DDTs对人体不构成健康威胁。组成特征分析表明,该地区水体中近期有林丹和三氯杀螨醇的使用。水体HCHs浓度在丰水期显著高于枯水期,不同时期DDTs浓度变化规律不明显。HCHs在丰水期趋向于以颗粒相的形式搬运、枯水期趋向于以溶解相的形式搬运；DDTs在水体中主要以颗粒相形式输运,以悬浮颗粒物为主要载体。水体OCPs空间分布特征都表现出,从大凌河流域流经河口及湿地地区向近海海域逐渐降低的趋势。大凌河口地区水体中颗粒有机质含量对控制OCPs在水体中的分布及其在两相中的分配起着重要的作用。
本论文第四部分对大凌河口地区沉积物污染特征进行研究。结果表明,沉积物中22种OCPs均有不同程度的检出,其中HCHs及其异构体和DDTs及其降解产物的检出率及残留量较高。表层沉积物OCPs浓度表现出,由大凌河流域流经河口及湿地地区至近海海域呈现出逐渐下降的趋势。采用210Pb放射性核素沉积柱定年方法,计算得出大凌河入海河口地区沉积物的平均沉积速率为1.12cm/a,本研究中沉积物柱芯的沉积年代可以追溯到1959年。基于210Pb定年的方法,建立了大凌河口地区柱状沉积物样品中HCHs和DDTs的垂直分布曲线与时间序列的对应关系。该地区沉积物中HCHs和DDTs主要来自于历史上的残留,但近二十多年来该地区环境中有林丹和三氯杀螨醇的输入。沉积物粒径大小是影响沉积物中OCPs残留与分布的重要因素。同时,表层沉积物中总有机碳含量对表层沉积物OCPs的残留量及其分布起着重要的作用：柱状沉积物OCPs残留量还与我国OCPs的生产使用及排放量和土壤残留量有关。根据沉积物风险评估标准,大凌河口地区沉积物中DDTs具有潜在生态风险,对该区域内生物会造成一定的生态危害。通过对OCPs在水体-沉积物间交换方向的初步预测可知,总体上,水环境中HCHs倾向于由水相向沉积相沉积；DDTs在水相与沉积相间趋于平衡且倾向于由沉积相向水相释放(湿地地区除外)。
Organochlorine Pesticides (OCPs) is a kind of typical Persistent Organic Pollutants (POPs) with high toxicity, semi-volatility, environmental persistence and bio-magnification. Nowadays, OCPs have become the worldwide environment problem due to serious adverse effects on organisms. In order to provide extensive information of residue, pollution, distribution, sources and influencing factor of22OCP compounds, multi-media environment (soil, water, sediment) samples were collected from2011to2012of Daling River Delta. All the research would get pollution status of OCPs in the Daling River Delta, apply as the scientific for pollutant control and management, and have great significance for protecting people's health and safety.
In the first part of this thesis, gridded usage inventories of OCPs in Daling River Basin was established, and then based on which, the OCPs emission and residue are calculated. With the supporting of usage data, HCHs and DDTs usage inventory was allocated to a grid system with1/4°longitude by1/6°latitude resolution, which was established from Geographic Information System (GIS) and Access Database System. The total usage of HCHs and DDTs were estimated to be approximately18kt and910t between1952and1984. On the base of usage inventory, SGPERM model was application for calculating emission and residue. The total emission of HCHs and DDTs between1952and1984were5600t and510t. The residue of HCHs and DDTs were2.2t and10.2t in the year of2010.
In the second part of this thesis, pollution characteristics of OCPs in soil of Linghai city were studied. The research shows that the22OCPs were detected with various in content in all the soil samples. HCHs and DDTs concentrations were detected with the high detection rates and residues. The results indicate that HCHs concentration in all soil samples and most DDTs concentration of soil samples were reached the first level of China's "Soil Environment Quality Standard"(GB15618-1995), HCHs pollution was generally slight ecological risk and DDTs pollution was potential ecological risk for some geobiont and local bird. Compositional analysis indicate that HCHs and DDTs residues in soil were mainly from history use, but some areas have new sources which were lindane and dicofol in recently. With the aid of multi-variate geostatistics and GIS, spatial distribution of OCPs was studied with results showing that OCPs varied greatly in spatial distribution between types.
In the third part of this thesis, pollution characteristics of OCPs in water of Daling River Delta were estimated. A total of22OCPs in surface water samplings were detected and HCHs and DDTs were the most dominant compounds in the water. Base on the health risk assessment, slight potential health risks of HCHs and DDTs in water may exist to organisms in Daling River Delta. There were lindane and dicofol input in recently years. The average concentration of HCHs in high water season was higher than that in low water season. HCHs in water presented in suspended particulate phase in high water season but dissolved phase in low water season. DDTs in water were mainly in suspended particulate phase. Geographical distributions of DDTs and HCHs from river area to coastal region were performed with the decreasing tendency. Total organic carbon in suspended particulate has influence on controlling OCPs'fate and transport in this area.
In the fourth part of this thesis, pollution characteristics of OCPs in sediment of Daling River Delta were discussed. The results shows hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) were the most frequently detected contaminants. The decreasing trends of OCPs concentrations from Daling River to estuary area to coastal region in surface sediment were observed. With the information about the vertical distribution of radioactive activity of210Pb in Daling River Delta, give average sedimentation rates were1.12cm/a and dated back to1959. Trough the study of the vertical distribution characteristics of OCPs in the sediment core, the pollution history of OCPs in Daling River Delta was discussed. Compositional analysis of HCHs and DDTs indicated that new sources were lindane and dicofol in recently twenty years. Grain size plays important role on the residue and distribution of OCPs in sediment. The total organic carbon in the surface sediments had good correlation with OCPs. The temporal trends of HCHs and DDTs concentrations in the sediment core were affected by application history, emission and soil residues. Additionally, base on the available sediment quality guidelines, slight potential health risks of DDTs may exist to organisms in Daling River Delta. Fugacity fraction between water and sediment in the river revealing a net flux from water to sediment of HCHs and a net flux from sediment to water of DDTs (except wetland).
本论文第一部分建立了大凌河流域有机氯农药历史使用清单,并在此基础上估算了该地区OCPs排放量与土壤残留量。在统计大量使用数据的基础上,本文利用地理信息系统和Access数据库,建立了我国大凌河流域1/4°经度×1/6°纬度分辨率的网格化的HCHs和DDTs的使用清单,使用清单从空间分布上量化了大凌河流域环境中HCHs和DDTs的来源。从1952～1984年间,大凌河流域HCHs和DDTs的使用量分别为18kt和910t。在使用清单的基础上,以SGPERM模型为工具,估算得出大凌河流域1960～2010年间环境中HCHs和DDTs的排放量为5600t和510t、土壤残留量在2010年分别为2.2t和10.2t。
本论文第二部分对大凌河中下游主要城市(凌海市)城区土壤中有机氯农药污染特征进行研究。结果表明：土壤中22种OCPs均有不同程度的检出,其中HCHs及其异构体和DDTs及其降解产物的检出率及残留量较高。土壤HCHs残留量均符合中国一级土壤标准(GB15618-1995),生态风险较低；部分土壤样品DDTs含量超出中国一级土壤标准,对当地土壤生物和鸟类具有一定的潜在生态风险。采用异构体比值法对土壤中HCHs和DDTs的来源进行初步判定,表明该地区土壤中HCHs和DDTs主要来自于历史上的残留,但近期部分地区有林丹和三氯杀螨醇的使用。表层土壤有机氯农药残留量受不同土地利用方式、上壤有机碳含量、土壤含水量和土壤粘粒含量影响显著(P<0.05)。利用多元地统计和地理信息系统GIS (Geographic Information System)相结合的分析方法,对凌海地区OCPs的空间分布进行研究表明,不同种类OCPs在研究区分布存在很大差异。
本论文第三部分对大凌河口地区水体中有机氯农药污染特征进行研究。结果显示：表层水体22种OCPs含量均有不同程度的检出,其中检出率和残留量较高的组分是HCHs和DDTS。经健康风险评价,该地区水体中HCHs和DDTs对人体不构成健康威胁。组成特征分析表明,该地区水体中近期有林丹和三氯杀螨醇的使用。水体HCHs浓度在丰水期显著高于枯水期,不同时期DDTs浓度变化规律不明显。HCHs在丰水期趋向于以颗粒相的形式搬运、枯水期趋向于以溶解相的形式搬运；DDTs在水体中主要以颗粒相形式输运,以悬浮颗粒物为主要载体。水体OCPs空间分布特征都表现出,从大凌河流域流经河口及湿地地区向近海海域逐渐降低的趋势。大凌河口地区水体中颗粒有机质含量对控制OCPs在水体中的分布及其在两相中的分配起着重要的作用。
本论文第四部分对大凌河口地区沉积物污染特征进行研究。结果表明,沉积物中22种OCPs均有不同程度的检出,其中HCHs及其异构体和DDTs及其降解产物的检出率及残留量较高。表层沉积物OCPs浓度表现出,由大凌河流域流经河口及湿地地区至近海海域呈现出逐渐下降的趋势。采用210Pb放射性核素沉积柱定年方法,计算得出大凌河入海河口地区沉积物的平均沉积速率为1.12cm/a,本研究中沉积物柱芯的沉积年代可以追溯到1959年。基于210Pb定年的方法,建立了大凌河口地区柱状沉积物样品中HCHs和DDTs的垂直分布曲线与时间序列的对应关系。该地区沉积物中HCHs和DDTs主要来自于历史上的残留,但近二十多年来该地区环境中有林丹和三氯杀螨醇的输入。沉积物粒径大小是影响沉积物中OCPs残留与分布的重要因素。同时,表层沉积物中总有机碳含量对表层沉积物OCPs的残留量及其分布起着重要的作用：柱状沉积物OCPs残留量还与我国OCPs的生产使用及排放量和土壤残留量有关。根据沉积物风险评估标准,大凌河口地区沉积物中DDTs具有潜在生态风险,对该区域内生物会造成一定的生态危害。通过对OCPs在水体-沉积物间交换方向的初步预测可知,总体上,水环境中HCHs倾向于由水相向沉积相沉积；DDTs在水相与沉积相间趋于平衡且倾向于由沉积相向水相释放(湿地地区除外)。
Organochlorine Pesticides (OCPs) is a kind of typical Persistent Organic Pollutants (POPs) with high toxicity, semi-volatility, environmental persistence and bio-magnification. Nowadays, OCPs have become the worldwide environment problem due to serious adverse effects on organisms. In order to provide extensive information of residue, pollution, distribution, sources and influencing factor of22OCP compounds, multi-media environment (soil, water, sediment) samples were collected from2011to2012of Daling River Delta. All the research would get pollution status of OCPs in the Daling River Delta, apply as the scientific for pollutant control and management, and have great significance for protecting people's health and safety.
In the first part of this thesis, gridded usage inventories of OCPs in Daling River Basin was established, and then based on which, the OCPs emission and residue are calculated. With the supporting of usage data, HCHs and DDTs usage inventory was allocated to a grid system with1/4°longitude by1/6°latitude resolution, which was established from Geographic Information System (GIS) and Access Database System. The total usage of HCHs and DDTs were estimated to be approximately18kt and910t between1952and1984. On the base of usage inventory, SGPERM model was application for calculating emission and residue. The total emission of HCHs and DDTs between1952and1984were5600t and510t. The residue of HCHs and DDTs were2.2t and10.2t in the year of2010.
In the second part of this thesis, pollution characteristics of OCPs in soil of Linghai city were studied. The research shows that the22OCPs were detected with various in content in all the soil samples. HCHs and DDTs concentrations were detected with the high detection rates and residues. The results indicate that HCHs concentration in all soil samples and most DDTs concentration of soil samples were reached the first level of China's "Soil Environment Quality Standard"(GB15618-1995), HCHs pollution was generally slight ecological risk and DDTs pollution was potential ecological risk for some geobiont and local bird. Compositional analysis indicate that HCHs and DDTs residues in soil were mainly from history use, but some areas have new sources which were lindane and dicofol in recently. With the aid of multi-variate geostatistics and GIS, spatial distribution of OCPs was studied with results showing that OCPs varied greatly in spatial distribution between types.
In the third part of this thesis, pollution characteristics of OCPs in water of Daling River Delta were estimated. A total of22OCPs in surface water samplings were detected and HCHs and DDTs were the most dominant compounds in the water. Base on the health risk assessment, slight potential health risks of HCHs and DDTs in water may exist to organisms in Daling River Delta. There were lindane and dicofol input in recently years. The average concentration of HCHs in high water season was higher than that in low water season. HCHs in water presented in suspended particulate phase in high water season but dissolved phase in low water season. DDTs in water were mainly in suspended particulate phase. Geographical distributions of DDTs and HCHs from river area to coastal region were performed with the decreasing tendency. Total organic carbon in suspended particulate has influence on controlling OCPs'fate and transport in this area.
In the fourth part of this thesis, pollution characteristics of OCPs in sediment of Daling River Delta were discussed. The results shows hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) were the most frequently detected contaminants. The decreasing trends of OCPs concentrations from Daling River to estuary area to coastal region in surface sediment were observed. With the information about the vertical distribution of radioactive activity of210Pb in Daling River Delta, give average sedimentation rates were1.12cm/a and dated back to1959. Trough the study of the vertical distribution characteristics of OCPs in the sediment core, the pollution history of OCPs in Daling River Delta was discussed. Compositional analysis of HCHs and DDTs indicated that new sources were lindane and dicofol in recently twenty years. Grain size plays important role on the residue and distribution of OCPs in sediment. The total organic carbon in the surface sediments had good correlation with OCPs. The temporal trends of HCHs and DDTs concentrations in the sediment core were affected by application history, emission and soil residues. Additionally, base on the available sediment quality guidelines, slight potential health risks of DDTs may exist to organisms in Daling River Delta. Fugacity fraction between water and sediment in the river revealing a net flux from water to sediment of HCHs and a net flux from sediment to water of DDTs (except wetland).
引文
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