钱塘江水体中多环芳烃的时空分布、污染来源及生物有效性
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摘要
地表水有机污染日益严重,主要污染物有多环芳烃(PAHs)、酚类化合物、有机氯农药和苯系物等,给饮用水安全带来一定风险,保护地面水尤其是饮用水源是当前面临的重大任务。准确掌握污染物浓度水平、污染来源及其生物可利用性可为控制地表水污染、保障饮用水安全提供理论依据。本文以钱塘江为代表,系统研究了饮用水源水、沉积物和近岸土壤中PAHs的浓度水平、时空分布及污染来源;估算了钱塘江河口段PAHs的输入输出通量;探讨了沉积物中PAHs的生物可利用性及影响因素,试图为保障饮用水安全提供一些有用的信息。论文取得了以下有价值的研究成果:
(1)钱塘江水、沉积物和近岸土壤中15种PAHs的总浓度范围分别为70.3-1844 ng/L、91.3-1835 ng/g dw和85.2-676.2 ng/g dw,平均浓度分别为288.2ng/L、326.6 ng/g dw和350.2 ng/g dw。PAHs浓度呈逐年升高趋势,冬季最高,夏季最低,城区江段高于农村江段。沉积物中Flur/(Flur+Py)和AN/(AN+Phen)比值分析表明钱塘江水体中PAHs主要来自石油类污染,但近年来燃烧产生的非石油源PAHs所占比重逐年增大。
(2)钱塘江河口段15种PAHs的输入通量约为21.83 t/yr,其中干沉降输入约为0.41 t/yr,湿沉降输入约为0.78 t/yr,地面径流输入约为8.50 t/yr,上游输入约为12.14 t/yr,下游输出通量约为13.49 t/yr,输入输出通量之差为8.34t/yr,输入通量高于输出通量,导致水体中PAHs浓度逐年升高。
(3)XAD-2辅助解吸法可评价沉积物中PAHs的生物可利用性。污染历史、来源基本相同的沉积物中生物不可利用的PAHs浓度与沉积物TOC含量呈线性正相关。
Surface water is polluted more seriously by organic contaminants.The protection of surface water resources is an important task for us.It is necessary to investigate the concentration,source and bioavailability of contaminants for the safety of drinking water.This dissertation selected Qiantang River as representative drinking water resource.The concentration,spatial and temporal distribution,and source of polycyclic aromatic hydrocarbons(PAHs)were characterized.Then,the input and output of PAHs in estuary section of Qiantang River were estimated. Furthermore,the bioavailability of PAHs in sediment were researched.The results provided valuable information for protection of drinking water resource.The main conclusions of this work were as follows:
(1)The total concentrations of 15 PAHs in water,sediment and soil from Qiantang River were ranged from 70.3 to 1844 ng/L,from 91.3 to 1835 ng/g dw and from 85.2 to 676.2 ng/g dw with the mean values of 288.2 ng/L,326.6 ng/g dw and 350.2 ng/g dw,respectively.The total concentrations of PAHs were increasing in recent years.The concentrations of PAHs were highest in winter and lowest in summer.The total concentrations of PAHs in city zones were higher than those in rural areas.Ratios of AN/(AN+Phen)and Flur/(Flur+Py)calculated suggested that PAHs in Qiantang River were mainly from petrogenic origin and the contribution of petrogenic PAHs was decreasing during the last two years.
(2)The input and output of PAHs in estuary section of Qiantang River were 21.83 t/yr and 13.49 t/yr,respectively.The input of PAHs was higher than output of PAHs,which caused the increase of concentrations of PAHs in Qiantang River.
(3)XAD-2 assisted desorption assay can be used to assess the bioavailability of PAHs in the sediment.Positive linear relationship was found between the non-bioavailable fraction of PAHs and TOC content when the samples were from the same origin.
(1)钱塘江水、沉积物和近岸土壤中15种PAHs的总浓度范围分别为70.3-1844 ng/L、91.3-1835 ng/g dw和85.2-676.2 ng/g dw,平均浓度分别为288.2ng/L、326.6 ng/g dw和350.2 ng/g dw。PAHs浓度呈逐年升高趋势,冬季最高,夏季最低,城区江段高于农村江段。沉积物中Flur/(Flur+Py)和AN/(AN+Phen)比值分析表明钱塘江水体中PAHs主要来自石油类污染,但近年来燃烧产生的非石油源PAHs所占比重逐年增大。
(2)钱塘江河口段15种PAHs的输入通量约为21.83 t/yr,其中干沉降输入约为0.41 t/yr,湿沉降输入约为0.78 t/yr,地面径流输入约为8.50 t/yr,上游输入约为12.14 t/yr,下游输出通量约为13.49 t/yr,输入输出通量之差为8.34t/yr,输入通量高于输出通量,导致水体中PAHs浓度逐年升高。
(3)XAD-2辅助解吸法可评价沉积物中PAHs的生物可利用性。污染历史、来源基本相同的沉积物中生物不可利用的PAHs浓度与沉积物TOC含量呈线性正相关。
Surface water is polluted more seriously by organic contaminants.The protection of surface water resources is an important task for us.It is necessary to investigate the concentration,source and bioavailability of contaminants for the safety of drinking water.This dissertation selected Qiantang River as representative drinking water resource.The concentration,spatial and temporal distribution,and source of polycyclic aromatic hydrocarbons(PAHs)were characterized.Then,the input and output of PAHs in estuary section of Qiantang River were estimated. Furthermore,the bioavailability of PAHs in sediment were researched.The results provided valuable information for protection of drinking water resource.The main conclusions of this work were as follows:
(1)The total concentrations of 15 PAHs in water,sediment and soil from Qiantang River were ranged from 70.3 to 1844 ng/L,from 91.3 to 1835 ng/g dw and from 85.2 to 676.2 ng/g dw with the mean values of 288.2 ng/L,326.6 ng/g dw and 350.2 ng/g dw,respectively.The total concentrations of PAHs were increasing in recent years.The concentrations of PAHs were highest in winter and lowest in summer.The total concentrations of PAHs in city zones were higher than those in rural areas.Ratios of AN/(AN+Phen)and Flur/(Flur+Py)calculated suggested that PAHs in Qiantang River were mainly from petrogenic origin and the contribution of petrogenic PAHs was decreasing during the last two years.
(2)The input and output of PAHs in estuary section of Qiantang River were 21.83 t/yr and 13.49 t/yr,respectively.The input of PAHs was higher than output of PAHs,which caused the increase of concentrations of PAHs in Qiantang River.
(3)XAD-2 assisted desorption assay can be used to assess the bioavailability of PAHs in the sediment.Positive linear relationship was found between the non-bioavailable fraction of PAHs and TOC content when the samples were from the same origin.
引文
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