渤海湾西岸典型持久性有机污染物的环境行为初步研究
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摘要
持久性有机污染物(POPs)是一类在环境中难降解、生物体内难代谢,具有很强的亲脂性,可以通过食物链富集,能够通过蒸发-冷凝等过程远距离传输的污染物,此类污染物毒性高,即使是微量水平也能对生态环境及人体健康产生显著不良影响。
本文采用硅胶净化法和凝胶渗透色谱法对环境样品进行净化、分离,应用GC-MS分析测定了环境样品中的历史性和新兴的典型痕量持久性有机污染物(多氯联苯(PCBs)、多溴联苯醚(PBDEs)、多环芳烃(PAHs)、有机氯农药(OCPs)等),并运用Preplink三联机全自动前处理仪建立了测定环境样品中OCPs的SPE-GPC-VAP全自动样品净化、分离和在线浓缩的前处理方法,结果较为满意。各目标物质的方法检出限分别为PAHs 0.02-0.20 ng/g;OCPs 0.02-1.97 ng/g;PCBs 1.01-10.0 pg/g;PBDEs 0.21-1.53 pg/g。
该研究对渤海湾西岸主要入海河流河口、典型潮间带和近岸海域的多种环境介质中PAHs、OCPs、PCBs和PBDEs等四类持久性有机污染物的污染现状、分布特征、污染来源进行了分析,初步研究了这四类污染物在渤海湾西岸的环境行为。研究结果表明:这四类典型持久性有机污染物在渤海湾西岸的分布趋势为入海河流>河口>潮间带>近岸海域,这表明有机污染物的污染主要是受陆域污染源影响。
在渤海湾西岸入海河流河口表层沉积物中PAHs总浓度范围为293.74-17 035.95 ng/g,多数以低环数(≤3环)PAHs占主导地位;OCPs总浓度范围为32.21-10 500.85 ng/g,其组成特征在不同的流域各不相同;PCBs的浓度范围在216.53-128 646.20 pg/g之间,多数河流沉积物中以10氯代PCBs为主要同类物,其次是6氯代和5氯代PCBs;PBDEs则在0-870.46 pg/g之间,多数河流以BDE28和47污染水平较高,在永定新河、大沽排污河以及北塘口BDE209也比较高。浮游动物体内PCBs和PBDEs的浓度比浮游植物高约1个数量级。OCPs、PCBs、PBDEs三类污染物质,在生物体内的含量均高于相对应的沉积物。
在4个典型潮间带表层沉积物中,PAHs的污染水平依次是歧口>驴驹河>滨海新区>海滨浴场;OCPs为歧口>滨海新区>海滨浴场>驴驹河;PCBs为滨海新区>歧口>海滨浴场>驴驹河;PBDEs则是滨海新区>海滨浴场>歧口>驴驹河。初步分析表明在潮间带表层沉积物中PAHs以3环PAHs为主要污染物,除滨海新区外OCPs以HCHs为主要污染物,沉积物中主要以4-6氯代PCBs为主,BDE209和BDE47在多数沉积物中占PBDEs比重大。在多数生物体中,这四类有机污染物的含量明显高于表层沉积物和间隙水,表明存在着生物富集效应。
对渤海湾西岸近岸海域表层沉积物中典型持久性有机污染物进行了初步的研究和分析。四类持久性有机污染物的污染水平依次分别为147.34-710.21 ng/g、19.13-242.62 ng/g,490.8-15 901.0 pg/g和0-126.21 pg/g。PAHs和PBDEs的总量分布大致是北部较高,中间较低,向南又升高的趋势,OCPs和PCBs的规律则不太明显。多环芳烃以低环数(≤3环)PAHs占主导地位;OCPs以HCHs为主要污染物;在绝大多数站位主要以3、4氯代PCBs为主,PBDEs中以BDE28、BDE209和BDE47为主要污染物。
对渤海湾西岸典型持久性有机污染物的源解析表明:PAHs来自石油和煤、木炭等燃料燃烧的复合污染,HCHs则主要是历史性的工业品六六六和林丹的混合污染,在多数区域DDT降解缓慢或者可能有新的DDT输入来源。PCBs是历史性的污染物,其在生物体内的污染水平较之沉积物高,说明PCBs具有较强的生物富集能力而且很难降解。PBDEs的污染受大气传输作用较大。对近岸海域沉积物中典型持久性有机污染物的风险评价表明:沉积物中PAHs、DDD、DDE和PCBs尚未对生物造成不利的影响,而DDTs可能对生物产生负效应,应引起注意。
Persistent Organic Pollutants (POPs) are chemical substances that persist in the environment, difficult to biological metabolism in body, highly lipophilic and toxic, bioaccumulate through the food web, can transported over long distances to regions where they have never been used, even if they are micro-level can also pose a risk of causing adverse effects to human health and ecological environment.
In this paper, the method of silica gel column and gel permeation chromatography has been adopted for cleanup and separation,and GC-MS has been used for analysis of the typical trace the historical and emerging persistent organic pollutants (polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), polycyclic aromatic hydrocarbons (PAHs), organochlorine pesticides (OCPs) in environmental samples. Meanwhile, developing automated purification, separation and in-line enrichment methods for OCPs in environmental samples using the SPE-GPC-VAP system. The determination limits of the methods for PAHs, OCPs, PCBs and PBDEs are 0.02 - 0.20 ng/g, 0.02 - 1.97 ng/g, 1.01 - 10.0 pg/g and 0.21 - 1.53 pg/g, respectively, which is available for detecting trace materials.
The pollution status, distribution and pollution sources of PAHs, OCPs, PCBs and PBDEs were analyzed for variety environmental samples in this article. The samples have been collected from the main river and estuarie, intertidal zone and inshore area about the west coast of Bohai bay. The environmental behavior of four pollutants in west coast of Bohai bay was to study, preliminary. The results show that the distribution of trends for the typical persistent organic pollutants in the Bohai Bay were as follow: rivers > estuaries > intertidal zone > inshore area, which indicated that the the pollution sources was land-based.
The total concentrations of PAHs range from 293.74 to 17 035.95 ng/g dw in the surface of sediments for the western coast river and estuaries of Bohai Bay, in sediments the PAHs dominating congeners is low cyclic compounds; The total concentrations of OCPs range from 32.21 - 10 500.85 ng/g dw, those characteristics of compositions were different in earch river; Total PCBs in the surface of sediments for the western coast river is 216.53 - 128 646.20 pg/g, in sediments congeners of PCBs 10 chlorines atoms is in the majority, follow by 5 and 6 chlorines atoms; Total PBDEs is 0 - 870.46 pg/g with high percentages of BDE28 and BDE47, in the Yongding New River, Dagu drainage River and Beitang estuaries BDE209 also higher. The level of PCBs and PBDEs in zooplankton body as 10 times as in phytoplankton. The concentration of OCPs, PCBs, PBDEs in vivo were higher than in sediments.
In the surface of sediments of four typical intertidal zone, the level of PAHs were as follows: Qikou > Luju river > Binhai New Area > beach bath; OCPs were as follow: Qikou > Binhai new area > beach bath > Luju river; The PCBs and PBDEs, respectively, were as follow: Binhai new area > Qikou > beach bath > Luju river; Binhai new area > beach bath > Qikou > Luju river. In sediments the PAHs dominating congeners is 3 cyclic compounds, and except Binhai new area, HCHs is the majority in sediment. The congeners of PCBs from 4 to 6 chlorines atoms are in the majority and the level of the BDE28 and BDE47 were higher in surface of sediments. The concentrations of four types of pollutant in most organisms were significantly higher than in the surface sediments and water, indicating that there is bioaccumulation effects.
The levels of four types of pollutant were ranging from 147.34 to 710.21 ng/g, 19.13 to 242 .62 ng/g, 490.8 to 15 901.0 pg/g, and 0 to 126.21 pg/g dw, respectively. PAHs and PBDEs were enriched mainly in the northern of inshore area, decreased in middle, the south has increased. The characteristic of OCPs and PCBs were not noticeable. In most of stations, the PAHs dominating congeners is low cyclic compounds, and HCHs is the majority for OCPs with congeners of PCBs from 3 to 4 chlorines atoms are in the majority. The level of the BDE28, BDE209 and BDE47 were higher.
The source analysis showed that both combustion from coal, charcoal, etc. and petroleum sources may account for PAHs loads in this area. HCHs are mainly historical mixture of pollution by HCB and lindane in industrial and DDT may be degradated slowly or have a new input source for in most regions. PCBs is a historic pollutants, compared with sediments, the organism was much more contaminated by PCBs, which indicate PCBs has a strong capacity of bio-concentration and difficult to degrade. The pollution of PBDEs came form atmospheric transport. The risk assessment shows that: PAHs, DDD, DDE and PCBs in sediment in inshore area can not caused adverse effects on biological but DDTs maybe have negative effects on biological.
本文采用硅胶净化法和凝胶渗透色谱法对环境样品进行净化、分离,应用GC-MS分析测定了环境样品中的历史性和新兴的典型痕量持久性有机污染物(多氯联苯(PCBs)、多溴联苯醚(PBDEs)、多环芳烃(PAHs)、有机氯农药(OCPs)等),并运用Preplink三联机全自动前处理仪建立了测定环境样品中OCPs的SPE-GPC-VAP全自动样品净化、分离和在线浓缩的前处理方法,结果较为满意。各目标物质的方法检出限分别为PAHs 0.02-0.20 ng/g;OCPs 0.02-1.97 ng/g;PCBs 1.01-10.0 pg/g;PBDEs 0.21-1.53 pg/g。
该研究对渤海湾西岸主要入海河流河口、典型潮间带和近岸海域的多种环境介质中PAHs、OCPs、PCBs和PBDEs等四类持久性有机污染物的污染现状、分布特征、污染来源进行了分析,初步研究了这四类污染物在渤海湾西岸的环境行为。研究结果表明:这四类典型持久性有机污染物在渤海湾西岸的分布趋势为入海河流>河口>潮间带>近岸海域,这表明有机污染物的污染主要是受陆域污染源影响。
在渤海湾西岸入海河流河口表层沉积物中PAHs总浓度范围为293.74-17 035.95 ng/g,多数以低环数(≤3环)PAHs占主导地位;OCPs总浓度范围为32.21-10 500.85 ng/g,其组成特征在不同的流域各不相同;PCBs的浓度范围在216.53-128 646.20 pg/g之间,多数河流沉积物中以10氯代PCBs为主要同类物,其次是6氯代和5氯代PCBs;PBDEs则在0-870.46 pg/g之间,多数河流以BDE28和47污染水平较高,在永定新河、大沽排污河以及北塘口BDE209也比较高。浮游动物体内PCBs和PBDEs的浓度比浮游植物高约1个数量级。OCPs、PCBs、PBDEs三类污染物质,在生物体内的含量均高于相对应的沉积物。
在4个典型潮间带表层沉积物中,PAHs的污染水平依次是歧口>驴驹河>滨海新区>海滨浴场;OCPs为歧口>滨海新区>海滨浴场>驴驹河;PCBs为滨海新区>歧口>海滨浴场>驴驹河;PBDEs则是滨海新区>海滨浴场>歧口>驴驹河。初步分析表明在潮间带表层沉积物中PAHs以3环PAHs为主要污染物,除滨海新区外OCPs以HCHs为主要污染物,沉积物中主要以4-6氯代PCBs为主,BDE209和BDE47在多数沉积物中占PBDEs比重大。在多数生物体中,这四类有机污染物的含量明显高于表层沉积物和间隙水,表明存在着生物富集效应。
对渤海湾西岸近岸海域表层沉积物中典型持久性有机污染物进行了初步的研究和分析。四类持久性有机污染物的污染水平依次分别为147.34-710.21 ng/g、19.13-242.62 ng/g,490.8-15 901.0 pg/g和0-126.21 pg/g。PAHs和PBDEs的总量分布大致是北部较高,中间较低,向南又升高的趋势,OCPs和PCBs的规律则不太明显。多环芳烃以低环数(≤3环)PAHs占主导地位;OCPs以HCHs为主要污染物;在绝大多数站位主要以3、4氯代PCBs为主,PBDEs中以BDE28、BDE209和BDE47为主要污染物。
对渤海湾西岸典型持久性有机污染物的源解析表明:PAHs来自石油和煤、木炭等燃料燃烧的复合污染,HCHs则主要是历史性的工业品六六六和林丹的混合污染,在多数区域DDT降解缓慢或者可能有新的DDT输入来源。PCBs是历史性的污染物,其在生物体内的污染水平较之沉积物高,说明PCBs具有较强的生物富集能力而且很难降解。PBDEs的污染受大气传输作用较大。对近岸海域沉积物中典型持久性有机污染物的风险评价表明:沉积物中PAHs、DDD、DDE和PCBs尚未对生物造成不利的影响,而DDTs可能对生物产生负效应,应引起注意。
Persistent Organic Pollutants (POPs) are chemical substances that persist in the environment, difficult to biological metabolism in body, highly lipophilic and toxic, bioaccumulate through the food web, can transported over long distances to regions where they have never been used, even if they are micro-level can also pose a risk of causing adverse effects to human health and ecological environment.
In this paper, the method of silica gel column and gel permeation chromatography has been adopted for cleanup and separation,and GC-MS has been used for analysis of the typical trace the historical and emerging persistent organic pollutants (polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), polycyclic aromatic hydrocarbons (PAHs), organochlorine pesticides (OCPs) in environmental samples. Meanwhile, developing automated purification, separation and in-line enrichment methods for OCPs in environmental samples using the SPE-GPC-VAP system. The determination limits of the methods for PAHs, OCPs, PCBs and PBDEs are 0.02 - 0.20 ng/g, 0.02 - 1.97 ng/g, 1.01 - 10.0 pg/g and 0.21 - 1.53 pg/g, respectively, which is available for detecting trace materials.
The pollution status, distribution and pollution sources of PAHs, OCPs, PCBs and PBDEs were analyzed for variety environmental samples in this article. The samples have been collected from the main river and estuarie, intertidal zone and inshore area about the west coast of Bohai bay. The environmental behavior of four pollutants in west coast of Bohai bay was to study, preliminary. The results show that the distribution of trends for the typical persistent organic pollutants in the Bohai Bay were as follow: rivers > estuaries > intertidal zone > inshore area, which indicated that the the pollution sources was land-based.
The total concentrations of PAHs range from 293.74 to 17 035.95 ng/g dw in the surface of sediments for the western coast river and estuaries of Bohai Bay, in sediments the PAHs dominating congeners is low cyclic compounds; The total concentrations of OCPs range from 32.21 - 10 500.85 ng/g dw, those characteristics of compositions were different in earch river; Total PCBs in the surface of sediments for the western coast river is 216.53 - 128 646.20 pg/g, in sediments congeners of PCBs 10 chlorines atoms is in the majority, follow by 5 and 6 chlorines atoms; Total PBDEs is 0 - 870.46 pg/g with high percentages of BDE28 and BDE47, in the Yongding New River, Dagu drainage River and Beitang estuaries BDE209 also higher. The level of PCBs and PBDEs in zooplankton body as 10 times as in phytoplankton. The concentration of OCPs, PCBs, PBDEs in vivo were higher than in sediments.
In the surface of sediments of four typical intertidal zone, the level of PAHs were as follows: Qikou > Luju river > Binhai New Area > beach bath; OCPs were as follow: Qikou > Binhai new area > beach bath > Luju river; The PCBs and PBDEs, respectively, were as follow: Binhai new area > Qikou > beach bath > Luju river; Binhai new area > beach bath > Qikou > Luju river. In sediments the PAHs dominating congeners is 3 cyclic compounds, and except Binhai new area, HCHs is the majority in sediment. The congeners of PCBs from 4 to 6 chlorines atoms are in the majority and the level of the BDE28 and BDE47 were higher in surface of sediments. The concentrations of four types of pollutant in most organisms were significantly higher than in the surface sediments and water, indicating that there is bioaccumulation effects.
The levels of four types of pollutant were ranging from 147.34 to 710.21 ng/g, 19.13 to 242 .62 ng/g, 490.8 to 15 901.0 pg/g, and 0 to 126.21 pg/g dw, respectively. PAHs and PBDEs were enriched mainly in the northern of inshore area, decreased in middle, the south has increased. The characteristic of OCPs and PCBs were not noticeable. In most of stations, the PAHs dominating congeners is low cyclic compounds, and HCHs is the majority for OCPs with congeners of PCBs from 3 to 4 chlorines atoms are in the majority. The level of the BDE28, BDE209 and BDE47 were higher.
The source analysis showed that both combustion from coal, charcoal, etc. and petroleum sources may account for PAHs loads in this area. HCHs are mainly historical mixture of pollution by HCB and lindane in industrial and DDT may be degradated slowly or have a new input source for in most regions. PCBs is a historic pollutants, compared with sediments, the organism was much more contaminated by PCBs, which indicate PCBs has a strong capacity of bio-concentration and difficult to degrade. The pollution of PBDEs came form atmospheric transport. The risk assessment shows that: PAHs, DDD, DDE and PCBs in sediment in inshore area can not caused adverse effects on biological but DDTs maybe have negative effects on biological.
引文
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