河流沉积物中重金属和农药的复合污染机理模型研究
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摘要
重金属和农药是水环境中较为常见的污染物,具有使用广泛、毒性大、排放量大、影响区域广的特点。近年来,随着工农业的迅速发展,重金属和有机农药在环境中的排放量、蓄积量越来越大。本文研究的铜和镉是两类不同性质的典型重金属污染物,近年来我国发生的重金属污染的公共事件很多与它们有关。随着农药的施用,残留的农药可以随着降雨进入河流、湖泊等水体,污染地表水,尤其是在我国东北地区。作为该区域广泛应用的除草剂和杀虫剂,阿特拉津和马拉硫磷的污染情况十分普遍,这两类污染物对环境和人类健康的危害日益凸显。它们在环境中共存而产生复合效应,可以大大改变某一或某些污染物的生理活性或毒性,对人类健康和水生态系统造成严重破坏。沉积物作为水环境中众多污染物的源和汇,对水环境中污染物的释放和迁移行为起着关键性作用。沉积物中的复合污染过程通常受到诸多因素的影响,包括外界影响因素(如环境条件)及内部因素(吸附质如沉积物组分、吸附剂如共存污染物)。各种影响因素对复合污染的影响是一个综合作用的过程,各因素间也可能存在相互制约、相互影响的关系。因此,研究重金属和有机污染物在沉积物上的复合吸附机理,明确作用于复合污染过程的各影响因素的贡献及相互关系,对受重金属、农药复合污染的河流进行环境修复有重要的理论指导意义。
本文选择镉、铜作为重金属污染物的代表,阿特拉津和马拉硫磷为典型农药的代表,以重金属存在条件下农药在水-沉积物体系中的复合污染机理为主要研究内容,着重考察不同类型影响因素对复合污染过程的作用及各因素间的关系,主要研究内容和成果包括：(1)采用BP人工神经网络、多元非线性回归等统计分析方法,应用中心复合实验设计等实验手段,研究多种重金属和农药在河流沉积物及其主要组分中的吸附规律及复合污染特征,建立污染物的吸附过程模型,明确重金属与农药的交互作用对各自吸附过程的影响,探索复合污染机理。所建BP人工神经网络模型经验证具有较好的预测能力和准确度,回归模型均通过显著性检验和拟合优度检验,利用所建模型不仅可以预测污染物的吸附规律,还能进一步明确沉积物组分、共存污染物间的交互作用及对吸附过程的相对贡献；(2)考察不同环境因子(包括温度、pH值、离子强度、曝气强度等)对农药和重金属复合污染的影响作用,并分别应用BP人工神经网络,多元非线性回归等方法,借助析因实验设计等实验手段,建立描述环境因子与污染物吸附量之间相互关系的模型。所建模型同样满足各类准确度检验,且通过预测可得出环境因子间的交互作用类型及对污染物吸附量的贡献；(3)将区间规划方法引入吸附过程模型中,假设分别以沉积物组分含量以及环境因子为考察对象的案例,建立基于不确定性条件下的吸附过程优化模型,确定沉积物主要组分以及环境因子与复合污染物吸附量之间的关系,通过优化得出两种案例中阿特拉津在沉积物上的最大吸附量范围,并对其产生的生态风险进行评价,得出阿特拉津对水环境中水生生物的生态风险并不显著；(4)综合考虑复合污染的几类影响因素对复合污染过程的作用,建立可以反映各因素间相互作用的结构方程模型,并比较因素影响作用的大小。综合模型建立后,可同时考察复合污染过程中,外部因素(环境因子)和内部因素(吸附剂沉积物组分和吸附质共存污染物)对复合污染过程所产生的作用。共存污染物对阿特拉津吸附的主要作用点在于沉积物组分,而环境条件对阿特拉津的直接作用远大于对沉积物组分的作用。本文研究内容可为复合污染修复,有针对性的减弱复合污染的影响程度,提出相应建设性意见和对策。
In recent years, emissions and volume of heavy metals and organic pesticides in the environment are increasing along with the rapid development of agriculture and industry. Because of pesticides's characteristics of high toxicity, emissions from large, wide influence range, they have become an important pollutants in water environment. The pollution of heavy metals to the environment catches people's eyes widely, their pollution prevention and control has been included in the "12th Five-Year" special planning. Copper and cadmium are two different types of typical heavy metal pollutants. In recent years, many public events about contaminated soil or sediment occurred in our country are associated with heavy metals. Atrazine and malathionis widely used in corn and vegetables in northeast China, and the pesticides can be applied to the soil by rainfall, runoff, and other ways to enter the rivers, lakes and other water bodies, resulting in the contamination of surface water. The harm of these two types of pollutants on the environment and human health has become prominent day by day. They always co-exist in the environment and produce a composite effect, and could significantly alter the physiological activity or toxic of one or some of the pollutants. They will cause serious damage to human health and aquatic ecosystems. As sources and sinks of many pollutants in the water environment, sediments play a significant role in the release and migration behavior of pollutants in the water environment. The composite pollution process in sediment is usually influenced by many factors, including external factors (such as environmental conditions) and internal factors (adsorbate such as sediment components, and adsorbents such as coexisted pollutants). The impact of various factors affecting the composite pollution is a process of comprehensive roles. It might presents increasingly influent relationship among the factors. Therefore, it is important to study the composite adsorption mechanism of heavy metals and organic pollutants in sediment, to clear contribution and mutual relations of each factor in the process of combined pollution. This study will be benefit for understanding the theoretical significance of composite ecological restoration in polluted rivers contaminanted by heavy metals and pesticides.
In this paper, mechanism of combined pollution among heavy metals (cadmium, copper) and pesticides (atrazine, malathion) in river sediments-water system were investigated. Effect of different types of influencing factors on the process of combined pollution and their relationship were studied from different angles, mainly including:(1) artificial neural networks, multiple nonlinear regression and central composite experimental design were used to simulate the adsorption process of pollutants. The established BP models have been proven to have good predictive ability and accuracy, and the regression models have all passed the test of significance and goodness of fit test. This paper established an adsorption mechanism for prediction model, we also use a complex system to clear on the adsorption of atrazine adsorption mechanism of the establishment of the model discussed in atrazine under different conditionsthe strength and type of interaction effects of heavy metals from different coexisting;(2) Effect of different environmental factors (including temperature, pH, ion strength and aeration intensity) on combined pollution among pesticides and heavy metals were investigated. Artificial neural networks, multiple nonlinear regression and factorial experimental design were used to build a model to describe the relationship among environmental factors and atrazine adsorption. Interaction among co-exsited pollutants and environmental factors was also described by this model;(3) Interval programming was introduced into the adsorption process model. It is assumed that the cases were the subject for examination of the sediment components content as well as environmental factors, and the adsorption process model was established based on conditions of uncertainty. Relationship between sediment major components and the adsorption amount of pollutants was determined derived by the model and scope of atrazine maximum adsorption capacity in the two cases were educed by optimizing the models so that the ecological risk of atrazine could be evaluated, and the evaluated results showed that ecological risk of atrazine to aquatic organisms was not signifisant;(4) Considering effect of different types of influencing factors on combined pollution, the structural equation model which could reflect the interaction among various factors was established, and the role of factors were obtained. Comprehensive model can examine the combined pollution process, the role of external factors (environmental factors) and internal factors (adsorbent sediment (components) and adsorbate (coexistence pollutants) combined pollution process. The main role on atrazine adsorption of coexisted pollutants lies in sediments compounds, and environmental conditions on atrazine is much larger than the direct effect of the sediment fractions. This paper surposed corresponding constructive comments and countermeasures on combined pollution repair, weakening the impact of the combined pollution.
本文选择镉、铜作为重金属污染物的代表,阿特拉津和马拉硫磷为典型农药的代表,以重金属存在条件下农药在水-沉积物体系中的复合污染机理为主要研究内容,着重考察不同类型影响因素对复合污染过程的作用及各因素间的关系,主要研究内容和成果包括：(1)采用BP人工神经网络、多元非线性回归等统计分析方法,应用中心复合实验设计等实验手段,研究多种重金属和农药在河流沉积物及其主要组分中的吸附规律及复合污染特征,建立污染物的吸附过程模型,明确重金属与农药的交互作用对各自吸附过程的影响,探索复合污染机理。所建BP人工神经网络模型经验证具有较好的预测能力和准确度,回归模型均通过显著性检验和拟合优度检验,利用所建模型不仅可以预测污染物的吸附规律,还能进一步明确沉积物组分、共存污染物间的交互作用及对吸附过程的相对贡献；(2)考察不同环境因子(包括温度、pH值、离子强度、曝气强度等)对农药和重金属复合污染的影响作用,并分别应用BP人工神经网络,多元非线性回归等方法,借助析因实验设计等实验手段,建立描述环境因子与污染物吸附量之间相互关系的模型。所建模型同样满足各类准确度检验,且通过预测可得出环境因子间的交互作用类型及对污染物吸附量的贡献；(3)将区间规划方法引入吸附过程模型中,假设分别以沉积物组分含量以及环境因子为考察对象的案例,建立基于不确定性条件下的吸附过程优化模型,确定沉积物主要组分以及环境因子与复合污染物吸附量之间的关系,通过优化得出两种案例中阿特拉津在沉积物上的最大吸附量范围,并对其产生的生态风险进行评价,得出阿特拉津对水环境中水生生物的生态风险并不显著；(4)综合考虑复合污染的几类影响因素对复合污染过程的作用,建立可以反映各因素间相互作用的结构方程模型,并比较因素影响作用的大小。综合模型建立后,可同时考察复合污染过程中,外部因素(环境因子)和内部因素(吸附剂沉积物组分和吸附质共存污染物)对复合污染过程所产生的作用。共存污染物对阿特拉津吸附的主要作用点在于沉积物组分,而环境条件对阿特拉津的直接作用远大于对沉积物组分的作用。本文研究内容可为复合污染修复,有针对性的减弱复合污染的影响程度,提出相应建设性意见和对策。
In recent years, emissions and volume of heavy metals and organic pesticides in the environment are increasing along with the rapid development of agriculture and industry. Because of pesticides's characteristics of high toxicity, emissions from large, wide influence range, they have become an important pollutants in water environment. The pollution of heavy metals to the environment catches people's eyes widely, their pollution prevention and control has been included in the "12th Five-Year" special planning. Copper and cadmium are two different types of typical heavy metal pollutants. In recent years, many public events about contaminated soil or sediment occurred in our country are associated with heavy metals. Atrazine and malathionis widely used in corn and vegetables in northeast China, and the pesticides can be applied to the soil by rainfall, runoff, and other ways to enter the rivers, lakes and other water bodies, resulting in the contamination of surface water. The harm of these two types of pollutants on the environment and human health has become prominent day by day. They always co-exist in the environment and produce a composite effect, and could significantly alter the physiological activity or toxic of one or some of the pollutants. They will cause serious damage to human health and aquatic ecosystems. As sources and sinks of many pollutants in the water environment, sediments play a significant role in the release and migration behavior of pollutants in the water environment. The composite pollution process in sediment is usually influenced by many factors, including external factors (such as environmental conditions) and internal factors (adsorbate such as sediment components, and adsorbents such as coexisted pollutants). The impact of various factors affecting the composite pollution is a process of comprehensive roles. It might presents increasingly influent relationship among the factors. Therefore, it is important to study the composite adsorption mechanism of heavy metals and organic pollutants in sediment, to clear contribution and mutual relations of each factor in the process of combined pollution. This study will be benefit for understanding the theoretical significance of composite ecological restoration in polluted rivers contaminanted by heavy metals and pesticides.
In this paper, mechanism of combined pollution among heavy metals (cadmium, copper) and pesticides (atrazine, malathion) in river sediments-water system were investigated. Effect of different types of influencing factors on the process of combined pollution and their relationship were studied from different angles, mainly including:(1) artificial neural networks, multiple nonlinear regression and central composite experimental design were used to simulate the adsorption process of pollutants. The established BP models have been proven to have good predictive ability and accuracy, and the regression models have all passed the test of significance and goodness of fit test. This paper established an adsorption mechanism for prediction model, we also use a complex system to clear on the adsorption of atrazine adsorption mechanism of the establishment of the model discussed in atrazine under different conditionsthe strength and type of interaction effects of heavy metals from different coexisting;(2) Effect of different environmental factors (including temperature, pH, ion strength and aeration intensity) on combined pollution among pesticides and heavy metals were investigated. Artificial neural networks, multiple nonlinear regression and factorial experimental design were used to build a model to describe the relationship among environmental factors and atrazine adsorption. Interaction among co-exsited pollutants and environmental factors was also described by this model;(3) Interval programming was introduced into the adsorption process model. It is assumed that the cases were the subject for examination of the sediment components content as well as environmental factors, and the adsorption process model was established based on conditions of uncertainty. Relationship between sediment major components and the adsorption amount of pollutants was determined derived by the model and scope of atrazine maximum adsorption capacity in the two cases were educed by optimizing the models so that the ecological risk of atrazine could be evaluated, and the evaluated results showed that ecological risk of atrazine to aquatic organisms was not signifisant;(4) Considering effect of different types of influencing factors on combined pollution, the structural equation model which could reflect the interaction among various factors was established, and the role of factors were obtained. Comprehensive model can examine the combined pollution process, the role of external factors (environmental factors) and internal factors (adsorbent sediment (components) and adsorbate (coexistence pollutants) combined pollution process. The main role on atrazine adsorption of coexisted pollutants lies in sediments compounds, and environmental conditions on atrazine is much larger than the direct effect of the sediment fractions. This paper surposed corresponding constructive comments and countermeasures on combined pollution repair, weakening the impact of the combined pollution.
引文
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