硫丹在中国土壤大气中空间分布及传播的研究
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摘要
硫丹是全球性的污染物质,具有持久性有机污染物(POPs)的特性,已经被《斯德哥尔摩公约》列为POPs候选物质,并且极有可能在未来加入《斯德哥尔摩公约》名单。
为了有效的削减和控制环境中的硫丹,为切实贯彻履行《斯德哥尔摩公约》实施计划提供科学依据,需要弄清其环境来源,归趋和迁移转化规律。鉴于目前国际社会关于硫丹的环境来源和归趋的研究比较少,并且不够系统,本论文研究硫丹在我国土壤大气中空间分布和传播。本研究主要分四条主线进行：(1)在大量收集原始数据的基础上,建立我国硫丹高分辨率的网格化的使用清单；在使用清单的基础上,建立我国硫丹高分辨率的网格化的排放/残留以及大气/土壤浓度清单；(2)在全国范围内设置监测点,全面监测硫丹在我国土壤/大气中的浓度值；(3)使用土壤/大气中的监测浓度对所建立的我国硫丹高分辨率的网格化的土壤/大气浓度清单作出评估；(4)研究我国硫丹土壤/大气界面交换规律并对其空间分布特征成因进行深入探讨。
我国硫丹的使用始于1994年,到2004年,估计累计使用量为25700 t。在使用数据的基础上,利用地理信息系统(GIS)与Access数据库相结合的研究手段,建立了我国硫丹1/4°经度×1/6°纬度分辨率的网格化的使用清单。在使用清单的基础上,运用SGPERM模型建立了排放和残留清单,并且进一步建立了我国土壤和大气的浓度清单。
本研究于2005年起开展了我国大气土壤中硫丹同步监测项目,在全国建立土壤监测点141个,大气监测点92个,全面监测土壤大气中的硫丹。由于长期大量的使用,硫丹已经成为我国土壤大气中广泛存在的污染物质,并且在使用地区其土壤大气浓度往往高于其它地区。在土壤中,β-硫丹的浓度值要远远高于α-硫丹,而这一关系在大气中正好相反,说明α-硫丹易于挥发到大气,而β-硫丹易于残留于土壤。研究中发现,土壤中硫丹硫酸盐与其母体化合物——α-硫丹和β-硫丹之间具有很好的线性关系,并由此建立了土壤中这三种硫丹类化合物的多元线性回归方程,进而利用我国土壤浓度清单中α-硫丹和β-硫丹的浓度值作为输入数据,得到了我国土壤中硫丹硫酸盐的浓度清单。
为了评价本研究中清单与模型的质量,将土壤大气中硫丹的监测数据与清单中对应模拟值进行一系列对比分析。结果表明,不论是在土壤还是在大气中,监测值与模拟值之间都具有很好的一致性,从而证明了本研究中建立的硫丹的清单与模型的准确性和合理性。
在监测值与模拟值的基础上,利用逸度模型估算了硫丹在我国土壤-大气界面的交换通量趋势。从土气交换通量时间上的变化特征来看,α-硫丹在夏秋季呈现典型的一次排放特征,而冬季表现出二次排放特征；β-硫丹则全年表现出一次排放特征。从土气交换通量空间分布特征来看,我国中部、东部和东北地区可能是环境中硫丹的主要的汇。
Endosulfan has become a global challenge. Due to its properties of persistent organic pollutants (POPs), endosulfan has been listed as candidate substance as new POPs by the" Convention of Stockholm". It is highly possible that endosulfan will be formally added to the list of the POPs by "Convention of Stockholm" in the future.
In order to reduce the amount of endosulfan in the environment, it is necessary to study the source, pathway and migration of endosulfan. This paper investigates the space distribution and spread of endosulfan in soil and atmosphere, the paper will:(1) establish gridded usage inventories of endosulfan in China with a high resolution, based on which, the endosulfan inventories of emission/residue and air/soil concentrations in China with the same resolution are established. (2) Set up monitoring sites across China to monitor the concentration of endosulfan in soil and air. (3) Assess the endosulfan inventories with the help of endosulfan soil and air monitoring data. (4) Study the soil-air exchange of endosulfan and discuss the cause of space distribution in depth.
The use of endosulfan in China started in 1994, and the total usage was estimated to be approximately 25700 t between 1994 to 2004. With the supporting of usage data, endosulfan usage inventory was allocated to a grid system with 1/4°longitude by 1/6°latitude resolution, which was established from Geographic Information System (GIS) and Access Database System. On the base of usage inventory, SGPERM model was application for developing Chinese emission and residue inventories, and furthermore for Chinese soil and air concentration inventories.
A survey of Chinese soil and air concurrently monitoring program was started in 2005 from 141 soil and 92 air sampling sites, in order to monitoring endosulfan in Chinese soil and air. Endosulfan was universal in Chinese soil and air due to heavily and long-term usage, and the higher concentration was always found in the area of endosulfan application. In soil samples, the concentrations ofβ-endosulfan were observed much higher than a-endosulfan, and the results were contrary in air samples, which indicated a-endosulfan is glad to volatile andβ-endosulfan prefer to reside in soil. Significant correlation between endosulfan sulfate and its parent isomers reflected that the presence of endosulfan sulfate is originated from its parent isomers. Based on multiple linear regression model, inventories of endosulfan sulfate in Chinese agricultural soil are established.
In order to assess the data derived from inventories and models, comparisons between field measurements and modeling results were performed. Significant correlations were found between the modeled and monitoring endosulfan concentrations, the good agreement lends credibility to modeling results.
An exchange flux trend of endosulfan between soil and air in China has been calculated by fugacity model based on measured data and simulated data. The change of exchange flux against time shows thatα-endosulfan is characteristic of primary emission in summer/autumn and secondary emission in winter.β-endosulfan features primary emission during the year. The change of exchange flux against space shows that the soil in central, estern and northeastern China is the major fate of endosulfan.
为了有效的削减和控制环境中的硫丹,为切实贯彻履行《斯德哥尔摩公约》实施计划提供科学依据,需要弄清其环境来源,归趋和迁移转化规律。鉴于目前国际社会关于硫丹的环境来源和归趋的研究比较少,并且不够系统,本论文研究硫丹在我国土壤大气中空间分布和传播。本研究主要分四条主线进行：(1)在大量收集原始数据的基础上,建立我国硫丹高分辨率的网格化的使用清单；在使用清单的基础上,建立我国硫丹高分辨率的网格化的排放/残留以及大气/土壤浓度清单；(2)在全国范围内设置监测点,全面监测硫丹在我国土壤/大气中的浓度值；(3)使用土壤/大气中的监测浓度对所建立的我国硫丹高分辨率的网格化的土壤/大气浓度清单作出评估；(4)研究我国硫丹土壤/大气界面交换规律并对其空间分布特征成因进行深入探讨。
我国硫丹的使用始于1994年,到2004年,估计累计使用量为25700 t。在使用数据的基础上,利用地理信息系统(GIS)与Access数据库相结合的研究手段,建立了我国硫丹1/4°经度×1/6°纬度分辨率的网格化的使用清单。在使用清单的基础上,运用SGPERM模型建立了排放和残留清单,并且进一步建立了我国土壤和大气的浓度清单。
本研究于2005年起开展了我国大气土壤中硫丹同步监测项目,在全国建立土壤监测点141个,大气监测点92个,全面监测土壤大气中的硫丹。由于长期大量的使用,硫丹已经成为我国土壤大气中广泛存在的污染物质,并且在使用地区其土壤大气浓度往往高于其它地区。在土壤中,β-硫丹的浓度值要远远高于α-硫丹,而这一关系在大气中正好相反,说明α-硫丹易于挥发到大气,而β-硫丹易于残留于土壤。研究中发现,土壤中硫丹硫酸盐与其母体化合物——α-硫丹和β-硫丹之间具有很好的线性关系,并由此建立了土壤中这三种硫丹类化合物的多元线性回归方程,进而利用我国土壤浓度清单中α-硫丹和β-硫丹的浓度值作为输入数据,得到了我国土壤中硫丹硫酸盐的浓度清单。
为了评价本研究中清单与模型的质量,将土壤大气中硫丹的监测数据与清单中对应模拟值进行一系列对比分析。结果表明,不论是在土壤还是在大气中,监测值与模拟值之间都具有很好的一致性,从而证明了本研究中建立的硫丹的清单与模型的准确性和合理性。
在监测值与模拟值的基础上,利用逸度模型估算了硫丹在我国土壤-大气界面的交换通量趋势。从土气交换通量时间上的变化特征来看,α-硫丹在夏秋季呈现典型的一次排放特征,而冬季表现出二次排放特征；β-硫丹则全年表现出一次排放特征。从土气交换通量空间分布特征来看,我国中部、东部和东北地区可能是环境中硫丹的主要的汇。
Endosulfan has become a global challenge. Due to its properties of persistent organic pollutants (POPs), endosulfan has been listed as candidate substance as new POPs by the" Convention of Stockholm". It is highly possible that endosulfan will be formally added to the list of the POPs by "Convention of Stockholm" in the future.
In order to reduce the amount of endosulfan in the environment, it is necessary to study the source, pathway and migration of endosulfan. This paper investigates the space distribution and spread of endosulfan in soil and atmosphere, the paper will:(1) establish gridded usage inventories of endosulfan in China with a high resolution, based on which, the endosulfan inventories of emission/residue and air/soil concentrations in China with the same resolution are established. (2) Set up monitoring sites across China to monitor the concentration of endosulfan in soil and air. (3) Assess the endosulfan inventories with the help of endosulfan soil and air monitoring data. (4) Study the soil-air exchange of endosulfan and discuss the cause of space distribution in depth.
The use of endosulfan in China started in 1994, and the total usage was estimated to be approximately 25700 t between 1994 to 2004. With the supporting of usage data, endosulfan usage inventory was allocated to a grid system with 1/4°longitude by 1/6°latitude resolution, which was established from Geographic Information System (GIS) and Access Database System. On the base of usage inventory, SGPERM model was application for developing Chinese emission and residue inventories, and furthermore for Chinese soil and air concentration inventories.
A survey of Chinese soil and air concurrently monitoring program was started in 2005 from 141 soil and 92 air sampling sites, in order to monitoring endosulfan in Chinese soil and air. Endosulfan was universal in Chinese soil and air due to heavily and long-term usage, and the higher concentration was always found in the area of endosulfan application. In soil samples, the concentrations ofβ-endosulfan were observed much higher than a-endosulfan, and the results were contrary in air samples, which indicated a-endosulfan is glad to volatile andβ-endosulfan prefer to reside in soil. Significant correlation between endosulfan sulfate and its parent isomers reflected that the presence of endosulfan sulfate is originated from its parent isomers. Based on multiple linear regression model, inventories of endosulfan sulfate in Chinese agricultural soil are established.
In order to assess the data derived from inventories and models, comparisons between field measurements and modeling results were performed. Significant correlations were found between the modeled and monitoring endosulfan concentrations, the good agreement lends credibility to modeling results.
An exchange flux trend of endosulfan between soil and air in China has been calculated by fugacity model based on measured data and simulated data. The change of exchange flux against time shows thatα-endosulfan is characteristic of primary emission in summer/autumn and secondary emission in winter.β-endosulfan features primary emission during the year. The change of exchange flux against space shows that the soil in central, estern and northeastern China is the major fate of endosulfan.
引文
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