广州大气中二噁英的浓度分布和几种典型二噁英排放源的初步研究
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摘要
持久性有机污染物具有难降解性、长距离迁移性和生物富集性，并且对生态环境存在潜在的危害，近年来已成为重要的国际化环境问题之一，二噁英就是持久性有机污染物的典型代表。了解二噁英的污染现状、排放源信息，以及以这些资料为基础建立起有效的污染对策和相应的法规政策等成为了当前国际社会最为紧迫的课题。本文对我国典型的南方城市广州大气中二噁英的环境行为(时空分布、来源、迁移和转化)进行了研究，并初步计算了广州居民的呼吸暴露风险；对影响广州大气质量的几种二噁英排放源进行初步的研究。
广州大气中二噁英的浓度水平受地区环境的影响较大，花都区、荔湾区、天河区和黄埔区大气颗粒物中二噁英的平均浓度(毒性当量浓度)分别为：3815fg／m~3(104.6 fg I-TEQ／m~3)、12777 fg／m~3(430.5 fg I-TEQ／m~3)、6963 fg／m~3(163.7 fg I-TEQ／m~3)和10953 fg／m~3(769.3 fg I-TEQ／m~3)；其浓度分布规律为：郊区<居民区<工业区。由于受到工业活动的影响，荔湾区和黄埔区是污染相对严重的区域。另外，本文对天河区大气进行了年度监测，结果表明其二噁英年平均浓度(毒性当量浓度)为：5295 fg／m~3(240.1 fg I-TEQ／m~3)。天河区大气中二噁英的浓度在温度高的季节比较低，在温度低的季节较高。
广州大气中二噁英的分布模式较为稳定，OCDF、OCDD、1，2，3，4，6，7，8-HpCDF和1，2，3，4，6，7，8-HpCDD四种化合物的浓度相对较高，其贡献之和超过总浓度的50％；2，3，4，7，8-PeCDF是所有单体中对总毒性当量贡献最大的一个，其范围为25％-40％。稳定的分布模式表明各地区的污染源相对固定，并且不具有季节性，各区域的排放源和区域的性质及功能相关，同时直接影响各区域的空气质量。
广州大气中二噁英在气相中所占的比例随氯原子数的增加而降低，四氯代的两种化合物大部分分配在气相，其范围为30％-100％；约有50％的五氯代二噁英分布在气相；六到八氯代的二噁英基本分布在颗粒相，气相中的比例一般不超过20％。
比较广州四城区呼吸暴露风险和日摄入量，荔湾区居民的暴露风险最大，尤其是儿童，其日摄入量为4.1 pg I-TEQ／kg／day，该值已经超过世界卫生组织规定的日摄入量的耐受范围。在天河区污染较为严重的日子里，居民的日摄入量也可能超过世界卫生组织的规定，例如：2005年1月6日，天河区成人和儿童的日摄入量分别为：3.2 pg I-TEQ／kg／day和4.3 pg I-TEQ／kg／day。如果存在特殊的污染，该地区居民的健康也会受到威胁。
通过对几种二噁英排放源的初步研究表明：电子垃圾焚烧，餐饮废气和汽车尾气都是广东地区潜在的二噁英排放源，后两种则是广州市的二噁英排放源。三种源的排放浓度(毒性当量)分别为：135666 fg／m~3(7509.5 fg I-TEQ／m~3)；17826fg／m~3(1821.1 fg I-TEQ／m~3)；5176 fg／m~3(251.8 fg I-TEQ／m~3)。电子垃圾焚烧不仅是溴代二噁英的重要排放源，同时也是氯代二噁英的重要排放源，对周围地区大气环境影响很大。由于燃烧材料，燃烧条件和燃烧程度等的不同，二噁英在三种排放源的气固分配比例有所不同。在餐饮废气和汽车尾气中，超过90％的二噁英集中在颗粒相上；电子垃圾焚烧废气中，超过30％的二噁英集中在气相，二噁英在气相中的比例随氯原子数的增加而降低。
As a typical representative of persistent organic pollutants, PCDD/Fs are of widely concerned due to their persistence, transportation, bioaccumulation and toxicity to biota. Consequently, investigation on level and emission sources of these pollutants as well as establishment of effective prevention measurement and legislation are hot global topics. In this thesis, atmospheric PCDD/Fs of Guangzhou, a typical southern city, was studied for environmental action (temporal and spatial distribution, sources, transportation and transformation). In addition, human risks of PCDD/Fs via inhalation were assessed. Moreover, some PCDD/Fs emission sources impacting on Guangzhou atmospheric quality were investigated preliminarily.
The levels of atmospheric PCDD/Fs in Guangzhou were associated with regional environment. The mean concentrations (I-TEQ values) for Huadu district, Liwan district, Tianhe district and Huangpu district were 3815 fg/m~3 (104.6 fg I-TEQ/m~3), 12777 fg/m~3 (430.5 fg I-TEQ/m~3), 6963 fg/m~3 (163.7 fg I-TEQ/m~3) and 10953 fg/m~3 (769.3 fg I-TEQ/m~3), respectively. The concentration distribution trend is suburb < residential area < industrial area. Liwan district and Huangpu district are seriously polluted areas due to industrial activities. On the other hand, after annual monitoring of atmosphere at Tianhe district, the PCDD/Fs annual concentration (I-TEQ value) was 5295 fg/m~3 (240.1 fg I-TEQ/m~3). The concentration of atmospheric PCDD/Fs for Tianhe district was low in high temperature season, and high in low temperature season.
The congener profile of atmospheric PCDD/Fs in Guangzhou was steady. The concentrations of OCDF, OCDD, 1,2,3,4,6,7,8-HpCDF and 1,2,3,4,6,7,8-HpCDD were relatively high, which accounting for more than 50% to total concentration. The contribution of 2,3,4,7,8-PeCDF to total I-TEQ was predominant with a range of 25%-40%. Steady congener profile suggested that the emission sources of PCDD/Fs in each area were fixed and no seasonal influence was observed. Emission sources of districts had correlation with their regional characteristic and function, which affected directly on regional atmospheric quality.
The percentage of the different PCDD/Fs congeners associated with gas phase was increased with the number of chlorine decrease, ranging from 30% to 100% for 4CDD/Fs, about 50% for 5CDD/Fs and <20% for 6-8CDD/Fs.
Of human risks via inhalation and daily intake in four districts in Guangzhou, inhabitants in Liwan district were highest. Especially for children, the daily intake for children was 4.1 pg I-TEQ/kg/day, and beyond the range for the tolerable daily intake of PCDD/Fs established by World Health Organization. In severely polluted day of Tianhe district, inhabitant's daily intake was possibly beyond the tolerable range. For example, the daily intakes for adults and children were 3.2 pg I-TEQ/kg/day and 4.3 pg I-TEQ/kg/day on Jan 6, 2006, respectively. Human health is probably threatened when there is some episode.
The results showed that electric waste combustion, cooking exhaust and vehicle exhaust were main potential PCDD/Fs emission sources for Guangdong province. The concentration (I-TEQ) of three PCDD/Fs emission sources were 135666 fg/m~3 (7509.5 fg I-TEQ/m~3), 17826 fg/m~3 (1821.1 fg I-TEQ/m~3) and 5176 fg/m~3 (251.8 fg I-TEQ/m~3), respectively. Electric waste combustion was not only important PBDD/Fs emission source, but also for PCDD/Fs, which could affect on ambient air quality. The gas-particle partitioning of PCDD/Fs emitted from three emission sources was different because of different burning material, burning condition and burning degree. More than 90% PCDD/Fs presented in particle phase in cooking exhaust and vehicle exhaust. However, more than 30% PCDD/Fs were in gas phase in electric waste combustion emission, the proportion of the different PCDD/Fs congeners associated in gas phase was increased with the number of chlorine decrease.
广州大气中二噁英的浓度水平受地区环境的影响较大，花都区、荔湾区、天河区和黄埔区大气颗粒物中二噁英的平均浓度(毒性当量浓度)分别为：3815fg／m~3(104.6 fg I-TEQ／m~3)、12777 fg／m~3(430.5 fg I-TEQ／m~3)、6963 fg／m~3(163.7 fg I-TEQ／m~3)和10953 fg／m~3(769.3 fg I-TEQ／m~3)；其浓度分布规律为：郊区<居民区<工业区。由于受到工业活动的影响，荔湾区和黄埔区是污染相对严重的区域。另外，本文对天河区大气进行了年度监测，结果表明其二噁英年平均浓度(毒性当量浓度)为：5295 fg／m~3(240.1 fg I-TEQ／m~3)。天河区大气中二噁英的浓度在温度高的季节比较低，在温度低的季节较高。
广州大气中二噁英的分布模式较为稳定，OCDF、OCDD、1，2，3，4，6，7，8-HpCDF和1，2，3，4，6，7，8-HpCDD四种化合物的浓度相对较高，其贡献之和超过总浓度的50％；2，3，4，7，8-PeCDF是所有单体中对总毒性当量贡献最大的一个，其范围为25％-40％。稳定的分布模式表明各地区的污染源相对固定，并且不具有季节性，各区域的排放源和区域的性质及功能相关，同时直接影响各区域的空气质量。
广州大气中二噁英在气相中所占的比例随氯原子数的增加而降低，四氯代的两种化合物大部分分配在气相，其范围为30％-100％；约有50％的五氯代二噁英分布在气相；六到八氯代的二噁英基本分布在颗粒相，气相中的比例一般不超过20％。
比较广州四城区呼吸暴露风险和日摄入量，荔湾区居民的暴露风险最大，尤其是儿童，其日摄入量为4.1 pg I-TEQ／kg／day，该值已经超过世界卫生组织规定的日摄入量的耐受范围。在天河区污染较为严重的日子里，居民的日摄入量也可能超过世界卫生组织的规定，例如：2005年1月6日，天河区成人和儿童的日摄入量分别为：3.2 pg I-TEQ／kg／day和4.3 pg I-TEQ／kg／day。如果存在特殊的污染，该地区居民的健康也会受到威胁。
通过对几种二噁英排放源的初步研究表明：电子垃圾焚烧，餐饮废气和汽车尾气都是广东地区潜在的二噁英排放源，后两种则是广州市的二噁英排放源。三种源的排放浓度(毒性当量)分别为：135666 fg／m~3(7509.5 fg I-TEQ／m~3)；17826fg／m~3(1821.1 fg I-TEQ／m~3)；5176 fg／m~3(251.8 fg I-TEQ／m~3)。电子垃圾焚烧不仅是溴代二噁英的重要排放源，同时也是氯代二噁英的重要排放源，对周围地区大气环境影响很大。由于燃烧材料，燃烧条件和燃烧程度等的不同，二噁英在三种排放源的气固分配比例有所不同。在餐饮废气和汽车尾气中，超过90％的二噁英集中在颗粒相上；电子垃圾焚烧废气中，超过30％的二噁英集中在气相，二噁英在气相中的比例随氯原子数的增加而降低。
As a typical representative of persistent organic pollutants, PCDD/Fs are of widely concerned due to their persistence, transportation, bioaccumulation and toxicity to biota. Consequently, investigation on level and emission sources of these pollutants as well as establishment of effective prevention measurement and legislation are hot global topics. In this thesis, atmospheric PCDD/Fs of Guangzhou, a typical southern city, was studied for environmental action (temporal and spatial distribution, sources, transportation and transformation). In addition, human risks of PCDD/Fs via inhalation were assessed. Moreover, some PCDD/Fs emission sources impacting on Guangzhou atmospheric quality were investigated preliminarily.
The levels of atmospheric PCDD/Fs in Guangzhou were associated with regional environment. The mean concentrations (I-TEQ values) for Huadu district, Liwan district, Tianhe district and Huangpu district were 3815 fg/m~3 (104.6 fg I-TEQ/m~3), 12777 fg/m~3 (430.5 fg I-TEQ/m~3), 6963 fg/m~3 (163.7 fg I-TEQ/m~3) and 10953 fg/m~3 (769.3 fg I-TEQ/m~3), respectively. The concentration distribution trend is suburb < residential area < industrial area. Liwan district and Huangpu district are seriously polluted areas due to industrial activities. On the other hand, after annual monitoring of atmosphere at Tianhe district, the PCDD/Fs annual concentration (I-TEQ value) was 5295 fg/m~3 (240.1 fg I-TEQ/m~3). The concentration of atmospheric PCDD/Fs for Tianhe district was low in high temperature season, and high in low temperature season.
The congener profile of atmospheric PCDD/Fs in Guangzhou was steady. The concentrations of OCDF, OCDD, 1,2,3,4,6,7,8-HpCDF and 1,2,3,4,6,7,8-HpCDD were relatively high, which accounting for more than 50% to total concentration. The contribution of 2,3,4,7,8-PeCDF to total I-TEQ was predominant with a range of 25%-40%. Steady congener profile suggested that the emission sources of PCDD/Fs in each area were fixed and no seasonal influence was observed. Emission sources of districts had correlation with their regional characteristic and function, which affected directly on regional atmospheric quality.
The percentage of the different PCDD/Fs congeners associated with gas phase was increased with the number of chlorine decrease, ranging from 30% to 100% for 4CDD/Fs, about 50% for 5CDD/Fs and <20% for 6-8CDD/Fs.
Of human risks via inhalation and daily intake in four districts in Guangzhou, inhabitants in Liwan district were highest. Especially for children, the daily intake for children was 4.1 pg I-TEQ/kg/day, and beyond the range for the tolerable daily intake of PCDD/Fs established by World Health Organization. In severely polluted day of Tianhe district, inhabitant's daily intake was possibly beyond the tolerable range. For example, the daily intakes for adults and children were 3.2 pg I-TEQ/kg/day and 4.3 pg I-TEQ/kg/day on Jan 6, 2006, respectively. Human health is probably threatened when there is some episode.
The results showed that electric waste combustion, cooking exhaust and vehicle exhaust were main potential PCDD/Fs emission sources for Guangdong province. The concentration (I-TEQ) of three PCDD/Fs emission sources were 135666 fg/m~3 (7509.5 fg I-TEQ/m~3), 17826 fg/m~3 (1821.1 fg I-TEQ/m~3) and 5176 fg/m~3 (251.8 fg I-TEQ/m~3), respectively. Electric waste combustion was not only important PBDD/Fs emission source, but also for PCDD/Fs, which could affect on ambient air quality. The gas-particle partitioning of PCDD/Fs emitted from three emission sources was different because of different burning material, burning condition and burning degree. More than 90% PCDD/Fs presented in particle phase in cooking exhaust and vehicle exhaust. However, more than 30% PCDD/Fs were in gas phase in electric waste combustion emission, the proportion of the different PCDD/Fs congeners associated in gas phase was increased with the number of chlorine decrease.
引文
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