Ⅳ级逸度模型对典型有机污染物环境行为的动态模拟
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摘要
有机污染物的多介质环境行为,以及其对生态环境和人类健康的潜在风险性越来越受到各相关领域学者的关注。数学模拟也成为了探讨有机污染物环境行为的重要手段。Mackay等建立的逸度模型以其结构简单、整体性好等特点成为了模拟有机污染物环境行为的优秀模型之一。其中,Ⅳ级逸度模型由于其模拟的环境系统逼近真实环境,能够研究有机污染物的动态环境行为,得到了广泛的应用。Ⅳ级逸度模型的应用不仅可以大大提高研究效率,提供污染物在多介质环境中随时间变化的污染水平、迁移的定量结果,且对环境污染预测、生态风险评价和污染控制措施优选等具有重要意义。
本研究以六六六(HCHs)为对象污染物,应用Ⅳ级逸度模型研究了其在黄河下游流域的动态归趋。另外,根据Ⅳ级逸度模型的温度依附性,考察了松花江污染事故后,温度对硝基苯环境行为的影响。Ⅳ级逸度模型的应用不仅对认识对象污染物的环境行为有重要意义,也为今后研究其它有机污染物提供方法学基础。
通过建立Ⅳ级逸度模型,模拟了HCHs在1952～2010年间黄河下游流域的环境归趋。模型预测的HCHs浓度值与实测值吻和较好,大部分残差低于0.5个对数单位。模拟结果很好的反映了HCHs的浓度随大量的农业施用和其后禁用导致的变化情况。β-HCH由于极难降解逐渐成为了环境中HCHs的主要异构体。HCHs在相邻介质间主要的迁移过程包括空气-土壤的湿沉降,空气-水的气扩散和土壤-水的径流。灵敏度分析结果表明,HCHs在土壤中的降解速率常数,与主要来源相关的参数等对模型结果影响相对较大。不确定性分析结果表明预测的HCHs在环境各相中的浓度的变异系数范围是0.5～5.8。
通过建立具有温度依附性的Ⅳ级逸度模型,重点考察了温度T对其环境行为的影响。结果表明,模型的主要参数逸度容量和迁移系数与T呈负相关,T对硝基苯在大气中的污染水平影响较大。随着T的降低,污染物从大气向其他环境相富集。0℃条件下,事故发生后水体和大气中硝基苯浓度峰值可分别达到背景值的4.9倍和4.7倍。模型预测的硝基苯浓度值与实测值吻和较好。
The multimedia environmental behavior of organic pollutants and their exposure risk to the ecosystems and human health has become more and more concerned by the researchers. Mathematical simulation is an important method used in studying environmental behavior of the pollutants. The fugacity model established by Mackay et al proved to be one of the most excellent environmental models because it can give accurate, comprehensive and reliable simulating results despite of its simple structure. As one of fugacity model, LevelⅣfugacity model can dynamically simulate the environmental behavior of organic pollutants, and was widely used by many researchers. It's an effective tool to study their concentration levels, and transfer processes between adjacent compartments quantitatively, and the results of simulation are significant to environmental pollution prediction, ecological risk assessment and optimization of environmental pollution control measures.
LevelⅣfugacity model were applied to simulate the dynamic transfer and fate of HCHs. Dynamic model depending on temperature with fugacity approach not only described the fate of Persistent Organic Pollutants (POPs) in the environment, but also evaluated the influences of temperature on environmental fate of pollutants. A levelⅣfugacity model was also developed to simulate temperature effects on multimedia fate pollutants emitted from environmental accidents, using nitrobenzene released from the Songhua River pollution accident in late 2005 as a case. It is significant to learn about their environmental impacts, and provide environmental parameters and model framework for studying the fate of other organic pollutants.
A levelⅣfugacity model was established to simulate the fate and transfer of HCH isomers in the lower reach of the Yellow River basin, China, during 1952～2010. The predicted concentrations of HCHs are in good agreement with the observed ones, as indicated by the residual errors being generally lower than 0.5 logarithmic units. The effects of extensive agricultural application and subsequent prohibition of HCHs are reflected by the temporal variation of HCHs predicted by the model. The proportions of HCH isomers in the environment also changed with time due to their different physicochemical properties. Althoughβ-HCH is not the main component of the technical HCHs, it has become the most abundant isomer in the environment because of its persistence. The dominant transfer processes between the adjacent compartments were deposition from air to soil, air diffusion through the air-water interface and runoff from soil to water. Sensitivity analysis showed that degradation rate in soil and parameters related to major sources had the strongest influence on the model result. Results of Monte Carlo simulation indicated the overall uncertainty of model predictions, and the coefficients of variation of the estimated concentrations of HCHs in all the compartments ranged from 0.5 to 5.8.
A levelⅣfugacity model was developed to simulate temperature effects after the accident. The results of simulation show that with the decrease of temperature, the fugacity capacities and nitrobenzene transfer coefficients among different compartments increase. As temperature decreases, pollutants in air compartment tend to partition into the other condensed compartments. At 0℃, peak concentration of nitrobenzene in water and air can reach 4.9 and 4.7 times as high as their background concentrations, respectively. LevelⅣfugacity model was proved to be an efficient method to evaluate the influences of temperature on environmental fate of pollutants released from accidents.
本研究以六六六(HCHs)为对象污染物,应用Ⅳ级逸度模型研究了其在黄河下游流域的动态归趋。另外,根据Ⅳ级逸度模型的温度依附性,考察了松花江污染事故后,温度对硝基苯环境行为的影响。Ⅳ级逸度模型的应用不仅对认识对象污染物的环境行为有重要意义,也为今后研究其它有机污染物提供方法学基础。
通过建立Ⅳ级逸度模型,模拟了HCHs在1952～2010年间黄河下游流域的环境归趋。模型预测的HCHs浓度值与实测值吻和较好,大部分残差低于0.5个对数单位。模拟结果很好的反映了HCHs的浓度随大量的农业施用和其后禁用导致的变化情况。β-HCH由于极难降解逐渐成为了环境中HCHs的主要异构体。HCHs在相邻介质间主要的迁移过程包括空气-土壤的湿沉降,空气-水的气扩散和土壤-水的径流。灵敏度分析结果表明,HCHs在土壤中的降解速率常数,与主要来源相关的参数等对模型结果影响相对较大。不确定性分析结果表明预测的HCHs在环境各相中的浓度的变异系数范围是0.5～5.8。
通过建立具有温度依附性的Ⅳ级逸度模型,重点考察了温度T对其环境行为的影响。结果表明,模型的主要参数逸度容量和迁移系数与T呈负相关,T对硝基苯在大气中的污染水平影响较大。随着T的降低,污染物从大气向其他环境相富集。0℃条件下,事故发生后水体和大气中硝基苯浓度峰值可分别达到背景值的4.9倍和4.7倍。模型预测的硝基苯浓度值与实测值吻和较好。
The multimedia environmental behavior of organic pollutants and their exposure risk to the ecosystems and human health has become more and more concerned by the researchers. Mathematical simulation is an important method used in studying environmental behavior of the pollutants. The fugacity model established by Mackay et al proved to be one of the most excellent environmental models because it can give accurate, comprehensive and reliable simulating results despite of its simple structure. As one of fugacity model, LevelⅣfugacity model can dynamically simulate the environmental behavior of organic pollutants, and was widely used by many researchers. It's an effective tool to study their concentration levels, and transfer processes between adjacent compartments quantitatively, and the results of simulation are significant to environmental pollution prediction, ecological risk assessment and optimization of environmental pollution control measures.
LevelⅣfugacity model were applied to simulate the dynamic transfer and fate of HCHs. Dynamic model depending on temperature with fugacity approach not only described the fate of Persistent Organic Pollutants (POPs) in the environment, but also evaluated the influences of temperature on environmental fate of pollutants. A levelⅣfugacity model was also developed to simulate temperature effects on multimedia fate pollutants emitted from environmental accidents, using nitrobenzene released from the Songhua River pollution accident in late 2005 as a case. It is significant to learn about their environmental impacts, and provide environmental parameters and model framework for studying the fate of other organic pollutants.
A levelⅣfugacity model was established to simulate the fate and transfer of HCH isomers in the lower reach of the Yellow River basin, China, during 1952～2010. The predicted concentrations of HCHs are in good agreement with the observed ones, as indicated by the residual errors being generally lower than 0.5 logarithmic units. The effects of extensive agricultural application and subsequent prohibition of HCHs are reflected by the temporal variation of HCHs predicted by the model. The proportions of HCH isomers in the environment also changed with time due to their different physicochemical properties. Althoughβ-HCH is not the main component of the technical HCHs, it has become the most abundant isomer in the environment because of its persistence. The dominant transfer processes between the adjacent compartments were deposition from air to soil, air diffusion through the air-water interface and runoff from soil to water. Sensitivity analysis showed that degradation rate in soil and parameters related to major sources had the strongest influence on the model result. Results of Monte Carlo simulation indicated the overall uncertainty of model predictions, and the coefficients of variation of the estimated concentrations of HCHs in all the compartments ranged from 0.5 to 5.8.
A levelⅣfugacity model was developed to simulate temperature effects after the accident. The results of simulation show that with the decrease of temperature, the fugacity capacities and nitrobenzene transfer coefficients among different compartments increase. As temperature decreases, pollutants in air compartment tend to partition into the other condensed compartments. At 0℃, peak concentration of nitrobenzene in water and air can reach 4.9 and 4.7 times as high as their background concentrations, respectively. LevelⅣfugacity model was proved to be an efficient method to evaluate the influences of temperature on environmental fate of pollutants released from accidents.
引文
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