中国α-六六六土壤残留分布特征及源汇解析的数值模拟研究
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摘要
持久性有机污染物(POPs)是一类在环境中持久性存在,可以通过环境迁移和食物链富集,对人类健康和生态环境产生有害影响的化合物。对POPs源汇关系的空间识别以及形成原因的认识是从区域尺度,乃至全球尺度把握POPs污染转移趋向,并制定控制与削减措施的理论基础,但是目前我国缺乏在国家尺度上的对POPs源汇关系的系统研究。土壤是POPs的主要环境归趋相之一,大气传输是POPs迁移的主要方式,因此,本研究选择我国(不包括台湾省)1952-1984年间使用量最大的有机氯农药六六六(HCHs,POPs的一种)的主要成分α-HCH为研究对象,利用以土壤为主要关心环境介质的长期模拟(1952-2007年),探讨了在HCHs使用期间,α-HCH的土壤残留特征以及主要的影响因素;识别出在HCHs停止使用后,α-HCH的主要污染汇区,并利用清单分离模拟方法进行了定量分析。进而利用以大气为主要关心环境介质的短期模拟(2005年)和多年气象资料分析相结合的方式,讨论了HCHs停止使用后,α-HCH在我国(不包括台湾省)的源汇空间分布的成因。
为模拟α-HCH在我国环境中的长期迁移转化规律,开发了一个基于1/4°经度×1/6°纬度的网格化多介质环境模型。模型中考虑土壤、大气、水和底泥4类环境介质,包括迁移和传输2个模块。
模拟结果表明,在HCHs使用期间,土壤中α-HCH残留浓度主要受α-HCH使用强度和拌种、毒土方式使用比例的影响;在HCHs停止使用后,则主要受温度以及土壤有机碳含量、土壤孔隙率的影响。在HCHs使用期间,较深层土壤(20-50 cm)的α-HCH残留浓度约为浅层土壤(0-20cm)的10%;此后,浅层土壤中α-HCH残留浓度下降速度相对较快。到2000年,浅层土壤中的残留浓度略高于较深层土壤。
东北、华北、东南以及中北地区的α-HCH土壤残留均以本地源贡献为主。1952-2007年期间,华北和东南地区的本地源贡献率均在95%以上,2个地区余下贡献比例基本是互为影响;东北和中北地区的本地源贡献比例分别在76%-94%和82%-99%之间,均呈逐年下降趋势。南部地区的α-HCH通过大气传输对东北和中北地区影响最大,贡献比例呈逐年上升的趋势,到2007年分别为19%和18%。利用1985-2007年的贡献比例变化趋势曲线拟合得出,到2030年和2041年南部源分别对东北和中北地区的α-HCH土壤残留贡献比例将大于50%。虽然东北地区比华北地区离南部地区更远,但南部地区单位α-HCH使用量对东北地区土壤残留贡献约为华北地区的10倍。
利用CanMETOP大气传输模型得出,2005年7月份在东北地区大气中出现了高于历史使用量最大的东南地区的α-HCH浓度。通过对风向、气压和降水等气象资料分析得出东亚夏季风可以将东南地区的α-HCH传输到东北地区,且大气浓度在东北地区的低压区内因风速的降低而升高。通过湿沉降通量、土-气逸度比以及土壤残留负荷比分析,表明东亚夏季风不仅对我国东部地区夏季大气中的α-HCH浓度的时空分布具有显著影响,对东北地区土壤污染作用也十分显著。
结合40多年的气象资料分析得出每年夏季是我国东南地区的α-HCH通过大气传输到达东北地区的重要时段,且以7月份最为显著。7月份传输至东北地区的α-HCH会因该地区经常出现的低压而在大气中堆集升高,从而通过与这一现象紧密联系的降水以湿沉积的形式进入东北地区的地表环境。
Persistent Organic Pollutants (POPs) are a group of chemicals that persist in environment, bioaccumulate through the food web, and pose a risk of causing adverse effects to human health and the environment. POPs can reach regions where they have never been used or produced through long-range transport and threat the environment in the regions. Spatial identification of the relationship between sources and acceptors of POPs and understanding the causes of this relationship are the theoretical foundation to master the pollution trends of these chemicals on a regional or even a global scale, and make policies to control and reduce the pollution. This kind research on a national scale is lacking in China. While soil is one of the sink for POPs, and atmospheric transport is the most important pathway of many chemicals to undergo the long-range transport process.
Technical HCH, one of POPs, was the mostly used insecticide in China from 1952 to 1984, andα-HCH, the major component of technical HCH, was selected as the targeted chemical in this study. The objective of this thesis is to study the pattern of the soil residues ofα-HCH in Chinese soil, the process to cause this residue patterns, and thereafter the relationship between source-receptor of the chemical.
A multi-medium model has been developed based on a grid system with a 1/6°×1/4°latitude/longitude resolution to assessment long-period fate ofα-HCH in China environment. The model considers 4 matrixes, soil, air, water and sediment, and includes transfer and transport modules. The model was employed to simulate the transport and transfer ofα-HCH in 56 years from 1952 to 2007, to analyze the characteristics of its residues in soil during the use of technical HCH, to identify the major contaminated areas, and to quantify the contributions to these areas from different source regions by using inventory separation method. Both the temporal and spatial trends ofα-HCH residues in Chinese multi-media, soil in particular, were calculated by the model. The results of the modeled soil concentrations matched well with the measured data. The model result suggested thatα-HCH concentration pattern in soil in each grid cell was mainly affected by usage intensity and application modes of this chemical in the cell during the application period from 1952 and 1983, and was dominated by temperature, organic carbon content and porosity of soil after 1983.
To identify quantitatively the contribution of different sources in China to theα-HCH budget national wide, the numerical simulations were performed for different scenarios. The results showed southern source was the remarkable contribution toα-HCH soil residue in Northeastern and mid-North China. The importance of the southern source has been stronger and it was predicted that over 50% ofα-HCH in Northeastern and mid-Northern soil will come from the southern sources in 2030 and 2041.
The temporal and spatial pattern ofα-HCH air concentration in China in 2005 was simulated by atmospheric transport model CanMETOP and indicated that the transport ofα-HCH from southeast soil to northeast China mainly caused by East Asian monsoon occurred in summer, mainly in July. It was found that East Asian monsoon can carryα-HCH from soil in Southern China, and bring them to the Northeast, forming a much strong“pulse”ofα-HCH in the region with a air concentration even higher than that in the source region.
Analysis on the meteorologic data during 1965-2007 shows thatα-HCH in southeast region was carryed into northeast China by air transport in summer of every year and maily in July.α-HCH transported into Northeast was concentrated by cyclone or lower air pressure and deposited into the environment of land surface by precipitation in the region.
为模拟α-HCH在我国环境中的长期迁移转化规律,开发了一个基于1/4°经度×1/6°纬度的网格化多介质环境模型。模型中考虑土壤、大气、水和底泥4类环境介质,包括迁移和传输2个模块。
模拟结果表明,在HCHs使用期间,土壤中α-HCH残留浓度主要受α-HCH使用强度和拌种、毒土方式使用比例的影响;在HCHs停止使用后,则主要受温度以及土壤有机碳含量、土壤孔隙率的影响。在HCHs使用期间,较深层土壤(20-50 cm)的α-HCH残留浓度约为浅层土壤(0-20cm)的10%;此后,浅层土壤中α-HCH残留浓度下降速度相对较快。到2000年,浅层土壤中的残留浓度略高于较深层土壤。
东北、华北、东南以及中北地区的α-HCH土壤残留均以本地源贡献为主。1952-2007年期间,华北和东南地区的本地源贡献率均在95%以上,2个地区余下贡献比例基本是互为影响;东北和中北地区的本地源贡献比例分别在76%-94%和82%-99%之间,均呈逐年下降趋势。南部地区的α-HCH通过大气传输对东北和中北地区影响最大,贡献比例呈逐年上升的趋势,到2007年分别为19%和18%。利用1985-2007年的贡献比例变化趋势曲线拟合得出,到2030年和2041年南部源分别对东北和中北地区的α-HCH土壤残留贡献比例将大于50%。虽然东北地区比华北地区离南部地区更远,但南部地区单位α-HCH使用量对东北地区土壤残留贡献约为华北地区的10倍。
利用CanMETOP大气传输模型得出,2005年7月份在东北地区大气中出现了高于历史使用量最大的东南地区的α-HCH浓度。通过对风向、气压和降水等气象资料分析得出东亚夏季风可以将东南地区的α-HCH传输到东北地区,且大气浓度在东北地区的低压区内因风速的降低而升高。通过湿沉降通量、土-气逸度比以及土壤残留负荷比分析,表明东亚夏季风不仅对我国东部地区夏季大气中的α-HCH浓度的时空分布具有显著影响,对东北地区土壤污染作用也十分显著。
结合40多年的气象资料分析得出每年夏季是我国东南地区的α-HCH通过大气传输到达东北地区的重要时段,且以7月份最为显著。7月份传输至东北地区的α-HCH会因该地区经常出现的低压而在大气中堆集升高,从而通过与这一现象紧密联系的降水以湿沉积的形式进入东北地区的地表环境。
Persistent Organic Pollutants (POPs) are a group of chemicals that persist in environment, bioaccumulate through the food web, and pose a risk of causing adverse effects to human health and the environment. POPs can reach regions where they have never been used or produced through long-range transport and threat the environment in the regions. Spatial identification of the relationship between sources and acceptors of POPs and understanding the causes of this relationship are the theoretical foundation to master the pollution trends of these chemicals on a regional or even a global scale, and make policies to control and reduce the pollution. This kind research on a national scale is lacking in China. While soil is one of the sink for POPs, and atmospheric transport is the most important pathway of many chemicals to undergo the long-range transport process.
Technical HCH, one of POPs, was the mostly used insecticide in China from 1952 to 1984, andα-HCH, the major component of technical HCH, was selected as the targeted chemical in this study. The objective of this thesis is to study the pattern of the soil residues ofα-HCH in Chinese soil, the process to cause this residue patterns, and thereafter the relationship between source-receptor of the chemical.
A multi-medium model has been developed based on a grid system with a 1/6°×1/4°latitude/longitude resolution to assessment long-period fate ofα-HCH in China environment. The model considers 4 matrixes, soil, air, water and sediment, and includes transfer and transport modules. The model was employed to simulate the transport and transfer ofα-HCH in 56 years from 1952 to 2007, to analyze the characteristics of its residues in soil during the use of technical HCH, to identify the major contaminated areas, and to quantify the contributions to these areas from different source regions by using inventory separation method. Both the temporal and spatial trends ofα-HCH residues in Chinese multi-media, soil in particular, were calculated by the model. The results of the modeled soil concentrations matched well with the measured data. The model result suggested thatα-HCH concentration pattern in soil in each grid cell was mainly affected by usage intensity and application modes of this chemical in the cell during the application period from 1952 and 1983, and was dominated by temperature, organic carbon content and porosity of soil after 1983.
To identify quantitatively the contribution of different sources in China to theα-HCH budget national wide, the numerical simulations were performed for different scenarios. The results showed southern source was the remarkable contribution toα-HCH soil residue in Northeastern and mid-North China. The importance of the southern source has been stronger and it was predicted that over 50% ofα-HCH in Northeastern and mid-Northern soil will come from the southern sources in 2030 and 2041.
The temporal and spatial pattern ofα-HCH air concentration in China in 2005 was simulated by atmospheric transport model CanMETOP and indicated that the transport ofα-HCH from southeast soil to northeast China mainly caused by East Asian monsoon occurred in summer, mainly in July. It was found that East Asian monsoon can carryα-HCH from soil in Southern China, and bring them to the Northeast, forming a much strong“pulse”ofα-HCH in the region with a air concentration even higher than that in the source region.
Analysis on the meteorologic data during 1965-2007 shows thatα-HCH in southeast region was carryed into northeast China by air transport in summer of every year and maily in July.α-HCH transported into Northeast was concentrated by cyclone or lower air pressure and deposited into the environment of land surface by precipitation in the region.
引文
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