环渤海西部地区大气中的PAHs污染
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摘要
大气中的多环芳烃(PAHs,polycyclic aromatic hydrocarbons)污染长期以来受到研究人员和政府部门的广泛关注。环渤海西部地区人口密集,工农业发达,PAHs排放密度较高。在本研究中,结合传统的主动采样技术和自行开发的被动采样技术,对该地区大气中的气相和颗粒相的PAHs污染特征进行了观测分析,同时通过收集降尘对大气PAHs的沉降进行估算,利用轨迹方法对研究区域大气PAHs传输特征进行了初步探讨。所观测物种为除萘以外的15种USEPA优控PAHs。
环渤海西部地区大气中PAHs浓度为:主动采样(24 h四次)54～1000 ng/m(3298±425 ng/m3)、被动采样(四季度)237～1500 ng/m3(752±337 ng/m3),高出欧美发达国家城市大气浓度数倍乃至一个数量级以上,是近年来世界上大气PAHs浓度水平最高的地区之一。与其他研究结果不同,环渤海西部地区大气PAHs浓度的城乡差别并不显著,城乡比值仅为1.24,而城乡样点的PAHs水平均高于背景点3～6倍。农村高浓度的大气PAHs主要是由农村地区煤/生物质的低效燃烧带来的高水平PAHs排放有关。
主动采样和被动采样结果所得PAHs的气固比例均小于2,低于世界温带其他地区报道(一般> 4)。在大气PAHs的气固分配过程中,log KPM10与log pl0的线性回归斜率mr小于-1,此现象与其他研究报道(一般为-0.6～-1)不同,反映了分配中主导机制是元素碳的吸附作用而非有机碳的吸收作用。PAHs的气固分配对其在环境中的降解、沉降和传输等行为有重要影响。
比较各季节大气PAHs浓度可以发现,冬季浓度最高,秋季次之,而春夏季最低。气相PAHs的冬夏比值为2左右,主要与冬季煤和生物质较多的燃用有关,大气扩散条件也有一定影响;冬季颗粒相PAHs比夏季高一个量级左右,排放、大气扩散条件、温度降水的季节变化是影响颗粒相PAHs冬夏比值的重要因素。大气PAHs高值分布区主要集中在河北省东北和西南部,河北西北部和山东西北部普遍较低。PAHs的空间分布与局地排放强度、人口密度、GDP等参数有显著正相关关系。
选用特征比值FLA/(FLA+PYR)和IcdP/(IcdP+BghiP)进行判断,发现煤和生物质燃烧是本区域大气PAHs的主要来源,燃油源在非采暖期有一定贡献。利用USEPA的PMF模型将本区域PAHs来源归为工业煤/交通、秸秆、生活煤和薪柴/炼焦,相应的贡献率分别为16.7%、18.1%、24.0%、41.2%,解析结果与排放估算结果基本一致。
研究区域PAHs沉降通量为8.5±6.2μg/(m2.d),大于上世纪90年代初英国城市中观测结果。城市与农村站点的PAHs沉降通量无显著差别(比值为1.29),而高出背景点6倍左右,与大气PAHs浓度的城乡差别相似。中高分子量(FLA～BghiP)与低分子量PAHs(ACY～ANT)沉降通量的空间分布模式不同,前者与大气PAHs浓度的空间分布类似,而后者在河北西北部山区沉降通量较高。利用轨迹模型分析显示本区域PAHs大气输出的可能性在冬季最大。
Atmospheric PAH contamination is a matter of great public health concern of scientists and policy makers in China. The Western Watershed of Bohai Sea, a area with large population, highly developed agriculture and industry, was recently identified as one of the areas in China with very high emission density of PAHs. Using both traditional active sampling and passive sampling technique developed in our lab, atmospheric PAH concentrations in gaseous and particulate phases were measured for the Western Watershed of Bohai Sea. Air-to-surface deposition depositions were also measured and atmospheric transport was addressed. The individual PAHs analyzed in this study were 16 USEPA priority PAHs except naphthalene.
Atmospheric PAH concentrations in the study area were 54~1000 ng/m(3298±425 ng/m3)based on 24h active sampling, or 237~1500 ng/m3(752±337 ng/m3)based on the full season passive sampling, which were several times higher than those in many cities in developed countries. In fact, the Western Watershed of Bohai Sea was one of the regions with highest atmospheric PAH levels in the world. Interestingly, there was no significant difference in atmospheric PAHs between urban and rural sites with urban/rural ratio of only 1.24 in this study. This urban-rural pattern was quite different from all the other reports which revealed much higher PAHs levels in urban than rural areas. For the high PAH levels in the rural atmosphere in this area, low combustion efficiencies of coal/biomass were the major reasons, which resulted in very high PAHs emission factors.
The Gas/Particulate ratio (G/P) of atmospheric PAHs in the study area was less than 2 for both active and passive sampling results, which was rather lower compared to the other reports in temperate zone. The regression slopes of partitioning coefficient log KPM10 and log pl0 were steeper than -1, out of the range of -0.6 ~ -1 often observed in other places, which provided an evidence for the EC adsorption domination in G-P partitioning.
The PAH levels were highest in winter but lowest in summer and spring. The winter/summer ratios were ~2 and ~10 for gaseous and particulate PAHs, respectively. The seasonal variation of consumption of coal/biomass and meteorological conditions were major driven factors for the seasonality of gaseous PAHs, and temperature-dependent gas-particulate partitioning played a more important role in the seasonal variation of particulate PAHs. Relative higher atmospheric PAH concentrations were observed in southwest and northeast parts of Hebei province, and lower values were found in west of Hebei and northwest of Shandong. The spatial distributions of atmospheric PAHs were positive correlated with local emission, population density and GDP significantly.
Diagnostic ratios of FLA/(FLA+PYR)和IcdP/(IcdP+BghiP) were applied for qualitative source apportionment. The combustions of coal and biomass were the major sources of atmospheric PAHs and petroleum combustion was important in non-heating season. Using PMF model provided by USEPA, four sources, namely industrial coal/vehicular, straw, domestic coal, and wood/coke oven, contributed 16.7%, 18.1%, 24.0% and 41.2% of the total emission, respectively. Roughly, the apportionment results were in agreement with the PAHs emission inventory of this area.
The atmospheric deposition flux of PAHs was 8.5±6.2μg/(m2.d), higher than those of UK cities observed in early 1990s. Similar PAH deposition fluxes were found between urban and rural sites with a urban/rural ratio of 1.29, but approximately 6 times lower than those at baseline sites. The urban-rural trends of PAH deposition were in line with the pattern of atmospheric PAH concentrations. Different spatial distribution patterns in the depositions were revealed between high-molecular-weight (≥202) and low-molecular-weight (< 202) PAHs. The former followed similar spatial distribution pattern of atmospheric PAH concentrations, while relative higher fluxes of the latter were observed in northwest of Hebei. The possibilities of atmospheric outflow of PAHs were highest in winter based on the results of calculation of air mass trajectories.
环渤海西部地区大气中PAHs浓度为:主动采样(24 h四次)54～1000 ng/m(3298±425 ng/m3)、被动采样(四季度)237～1500 ng/m3(752±337 ng/m3),高出欧美发达国家城市大气浓度数倍乃至一个数量级以上,是近年来世界上大气PAHs浓度水平最高的地区之一。与其他研究结果不同,环渤海西部地区大气PAHs浓度的城乡差别并不显著,城乡比值仅为1.24,而城乡样点的PAHs水平均高于背景点3～6倍。农村高浓度的大气PAHs主要是由农村地区煤/生物质的低效燃烧带来的高水平PAHs排放有关。
主动采样和被动采样结果所得PAHs的气固比例均小于2,低于世界温带其他地区报道(一般> 4)。在大气PAHs的气固分配过程中,log KPM10与log pl0的线性回归斜率mr小于-1,此现象与其他研究报道(一般为-0.6～-1)不同,反映了分配中主导机制是元素碳的吸附作用而非有机碳的吸收作用。PAHs的气固分配对其在环境中的降解、沉降和传输等行为有重要影响。
比较各季节大气PAHs浓度可以发现,冬季浓度最高,秋季次之,而春夏季最低。气相PAHs的冬夏比值为2左右,主要与冬季煤和生物质较多的燃用有关,大气扩散条件也有一定影响;冬季颗粒相PAHs比夏季高一个量级左右,排放、大气扩散条件、温度降水的季节变化是影响颗粒相PAHs冬夏比值的重要因素。大气PAHs高值分布区主要集中在河北省东北和西南部,河北西北部和山东西北部普遍较低。PAHs的空间分布与局地排放强度、人口密度、GDP等参数有显著正相关关系。
选用特征比值FLA/(FLA+PYR)和IcdP/(IcdP+BghiP)进行判断,发现煤和生物质燃烧是本区域大气PAHs的主要来源,燃油源在非采暖期有一定贡献。利用USEPA的PMF模型将本区域PAHs来源归为工业煤/交通、秸秆、生活煤和薪柴/炼焦,相应的贡献率分别为16.7%、18.1%、24.0%、41.2%,解析结果与排放估算结果基本一致。
研究区域PAHs沉降通量为8.5±6.2μg/(m2.d),大于上世纪90年代初英国城市中观测结果。城市与农村站点的PAHs沉降通量无显著差别(比值为1.29),而高出背景点6倍左右,与大气PAHs浓度的城乡差别相似。中高分子量(FLA～BghiP)与低分子量PAHs(ACY～ANT)沉降通量的空间分布模式不同,前者与大气PAHs浓度的空间分布类似,而后者在河北西北部山区沉降通量较高。利用轨迹模型分析显示本区域PAHs大气输出的可能性在冬季最大。
Atmospheric PAH contamination is a matter of great public health concern of scientists and policy makers in China. The Western Watershed of Bohai Sea, a area with large population, highly developed agriculture and industry, was recently identified as one of the areas in China with very high emission density of PAHs. Using both traditional active sampling and passive sampling technique developed in our lab, atmospheric PAH concentrations in gaseous and particulate phases were measured for the Western Watershed of Bohai Sea. Air-to-surface deposition depositions were also measured and atmospheric transport was addressed. The individual PAHs analyzed in this study were 16 USEPA priority PAHs except naphthalene.
Atmospheric PAH concentrations in the study area were 54~1000 ng/m(3298±425 ng/m3)based on 24h active sampling, or 237~1500 ng/m3(752±337 ng/m3)based on the full season passive sampling, which were several times higher than those in many cities in developed countries. In fact, the Western Watershed of Bohai Sea was one of the regions with highest atmospheric PAH levels in the world. Interestingly, there was no significant difference in atmospheric PAHs between urban and rural sites with urban/rural ratio of only 1.24 in this study. This urban-rural pattern was quite different from all the other reports which revealed much higher PAHs levels in urban than rural areas. For the high PAH levels in the rural atmosphere in this area, low combustion efficiencies of coal/biomass were the major reasons, which resulted in very high PAHs emission factors.
The Gas/Particulate ratio (G/P) of atmospheric PAHs in the study area was less than 2 for both active and passive sampling results, which was rather lower compared to the other reports in temperate zone. The regression slopes of partitioning coefficient log KPM10 and log pl0 were steeper than -1, out of the range of -0.6 ~ -1 often observed in other places, which provided an evidence for the EC adsorption domination in G-P partitioning.
The PAH levels were highest in winter but lowest in summer and spring. The winter/summer ratios were ~2 and ~10 for gaseous and particulate PAHs, respectively. The seasonal variation of consumption of coal/biomass and meteorological conditions were major driven factors for the seasonality of gaseous PAHs, and temperature-dependent gas-particulate partitioning played a more important role in the seasonal variation of particulate PAHs. Relative higher atmospheric PAH concentrations were observed in southwest and northeast parts of Hebei province, and lower values were found in west of Hebei and northwest of Shandong. The spatial distributions of atmospheric PAHs were positive correlated with local emission, population density and GDP significantly.
Diagnostic ratios of FLA/(FLA+PYR)和IcdP/(IcdP+BghiP) were applied for qualitative source apportionment. The combustions of coal and biomass were the major sources of atmospheric PAHs and petroleum combustion was important in non-heating season. Using PMF model provided by USEPA, four sources, namely industrial coal/vehicular, straw, domestic coal, and wood/coke oven, contributed 16.7%, 18.1%, 24.0% and 41.2% of the total emission, respectively. Roughly, the apportionment results were in agreement with the PAHs emission inventory of this area.
The atmospheric deposition flux of PAHs was 8.5±6.2μg/(m2.d), higher than those of UK cities observed in early 1990s. Similar PAH deposition fluxes were found between urban and rural sites with a urban/rural ratio of 1.29, but approximately 6 times lower than those at baseline sites. The urban-rural trends of PAH deposition were in line with the pattern of atmospheric PAH concentrations. Different spatial distribution patterns in the depositions were revealed between high-molecular-weight (≥202) and low-molecular-weight (< 202) PAHs. The former followed similar spatial distribution pattern of atmospheric PAH concentrations, while relative higher fluxes of the latter were observed in northwest of Hebei. The possibilities of atmospheric outflow of PAHs were highest in winter based on the results of calculation of air mass trajectories.
引文
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