浙江沿海沉积物和海洋生物中持久性有机污染物及重金属的分析与研究
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摘要
浙江省位于中国的东南沿海，海岸线总长为6，321公里，拥有杭州湾、象山湾、三门湾和乐清湾四大港湾以及大小岛屿3，016座。区域内的舟山渔场是国内最大的渔场和国际著名的渔场之一。近二十年来，随着长三角地区经济的快速发展，浙江沿海受到了长江、钱塘江及江、浙、沪陆源入海污染影响，加上海洋养殖、捕捞及海洋运输等造成的污染，该海域的污染水平呈现逐年加重趋势。为研究浙江沿海水体的污染状况，我们对长江口、杭州湾及舟山海域沉积物和沿岸海洋生物体内的多氯联苯、多环芳烃、有机氯农药以及重金属的含量水平、分布特征、影响因素及生态风险进行研究和分析，得到以下结果：
1．建立了同时对海洋贝类中20种有机氯农药、28种多氯联苯和16种多环芳烃的同位素稀释气相色谱—离子阱质谱分析方法，确定了凝胶净化色谱的最佳组分收集时间和铝硅胶柱两种连续淋洗溶剂的体积。结果表明，多氯联苯、有机氯农药和多环芳烃各化合物的方法检出限分别为0.01-0.14，0.02～0.17和0.52～0.81 ng/g(湿重)，样品的加标回收率和相对标准偏差分别为：多氯联苯84.1％～120.2％，5.6～15.9％；多环芳烃62.3％～123.1％，8.7～20.5％；有机氯农药77.3％～127.5％，3.1～18.7％。
2．以所建立的分析方法对采自浙江沿海12个县(市)的贝类、鱼类和虾类等生物样品进行了有机氯农药、多氯联苯和多环芳烃含量的分析，结果表明：
生物体内有机氯农药的主要化合物是p，p′-DDE，p，p′-DDD，p，p′-DDT，γ-氯丹和α-氯丹。DDT／(DDE+DDD)比值判断结果表明：嵊泗、普陀、宁海、乐清、椒江和玉环等六个区域可能存在着DDT类农药或含DDT的农药新的来源。贝类中的多氯联苯以六氯代同族体为主要组成，其次分别为四氯代、五氯代、三氯代和七氯代。贝类中多环芳烃以高苯环数的为主，而龙头鱼和脊尾白虾体内的多环芳烃主要以低苯环数的二环和三环为主。
从生物种类来看，贝类体内多氯联苯、多环芳烃和有机氯农药水平明显高于龙头鱼和脊尾白虾，反映贝类对有机污染物具有较强的积蓄能力。区域分布特征表明，乐清贝类体内的多氯联苯和多环芳烃的含量较高，而嵊泗和普陀贝类有机氯农药和多环芳烃处于较高水平。除椒江龙头鱼多氯联苯含量较高外，各区域龙头鱼中有机氯农药和多环芳烃含量接近。宁海和玉环脊尾白虾有机氯和多氯联苯的含量较高，各区域脊尾白虾中的多环芳烃含量接近。
贝类、龙头鱼和脊尾白虾部分样品的DDTs超过欧盟、美国EPA和我国海洋生物标准的限值，其中贝类的超限值率为最高。致癌风险评价结果表明：生物体内有机污染物的EDI值均低于相对应的RfD和CBC值。生物体内的DDTs和HCHs的EDI值也远低于FAO／WHO推荐的ADI(可接受每日摄入量)。对浙江居民来说，目前食用贝类、龙头鱼和脊尾白虾不会对其构成致癌风险。
3．研究区域表层沉积物中多环芳烃、多氯联苯和有机氯农药这三类有机污染物的高值区均出现在长江口南支南汇嘴附近和杭州湾北岸。长江口北支口外海域沉积物中的含量明显低于南支附近海域。沉积物中有机污染物主要是受陆域污染源，特别是长江径流的影响。
长江口、杭州湾和舟山海区表层沉积物多环芳烃的组成规律相同，均为三环＞四环＞五环＞二环＞六环。多环芳烃主要来源于油类与木柴、煤的燃烧，而石油产品的泄漏排放也是其来源之一。沉积物中多氯联苯主要是以低氯代的多氯联苯同族体为主。而沉积物的DDT／(DDE+DDD)比值显示研究区域总体上没有DDT类农药新的输入来源。
沉积物中的有机碳是影响多环芳烃、多氯联苯和有机氯农药含量的主要因素。表层沉积物中多环芳烃、多氯联苯和有机氯农药具有长江径流来源的这一相同特征。
多环芳烃、有机氯农药和多氯联苯组分含量大部分低于美国NOAASQG的ER-L值，沉积物质量状况总体上处于良好的状态。长江口南支附近和杭州湾湾口部分沉积物中的芴浓度和半数以上站位DDTs含量已超过了ER-L值。研究区域沉积物中的多环芳烃、多氯联苯和有机氯农药(HCHs和DDTs)的含量总体上处于较低或中等水平。
4．研究区域中，表层沉积物主要组成类型为粉砂和粘土质粉砂。沉积物中的Cu、Cd、Cr、Fe和Ni的总量低于背景值；而杭州湾中部和长江口口内沉积物Pb、Zn和Mn高于背景值。在长江口区域，沉积物中重金属含量从长江口南支内向口外方向递减；杭州湾沉积物重金属亦有湾内向湾外方向降低的趋势，但湾中部沉积物重金属含量较高。沉积物中的重金属均未超出沉积物二类控制标准或ER-M、PEL值。陆源沉积物的颗粒粒径是影响沉积物重金属和有机碳水平的重要因素。研究区域沉积物可能具有相同来源或相似的输送和积累机理。沉积物中的Cr、Fe、Ni、Pb、Zn和Cu主要存在于残留态中，对环境污染的风险较低，而沉积物中的重金属Cd和Mn具有潜在的环境污染风险。
5．与国内外沿海区域相比较，浙江沿岸海域鱼类、贝类、虾类和头足类体内Cu、Pb、Zn、Cd、Hg和As的含量水平总体上处于较低的水平。其中，Zn和Cu元素的含量为最高，而其它重金属Pb、Cd、As和Hg含量相对较低。贝类对重金属元素的积累能力为最强，头足类次之，其次为虾类，而积累能力最弱的为鱼类。所研究的海洋生物未受到重金属的严重污染，但贝类的Cu和Cd，鱼类的As和Zn，以及虾类的As处于轻度污染水平。除贝类和虾类的重金属Cd和虾类的As含量超出了澳大利亚的“人体消费卫生标准”的限值外，其它重金属含量均低于食用限值，表明研究区域的海洋生物质量总体上处于良好的状态。
Zhejiang province is located in the southeast coastal areas of China, with the total coastline about 6,321 km in length. There are four bays, i.e. Hangzhou bay, Xiangshan harbour, Sanmen bay and Yueqing bay, and 3,016 islands in this area. The region also includes Zhoushan fishing ground, which is the largest one in China and an internationally important fishing ground that contains many actual and potential maricultural sites. In recent twenty years, with the rapid economic development of Changjiang Delta area, the coastal environment was increasingly influenced by pollutants from Changjiang River and Qiangtang River runoffs, and non-point land-based pollutants from Jiangsu, Zhejiang and Shanghai in addition to activities of marine aquaculture, fishing and shipping, etc. The status of environmental quality in the area is deteriorating in recent years. In this study, the levels, distribution features, impact factors and ecological risks of the persistent organic pollutants (POPs), i.e. polychlorinated biphenyls, polycyclic aromatic hydrocarbons and organochlorine pesticides, and heavy metals in surface sediments from Changjiang estuary, Hangzhou Bay and Zhoushan marine areas and marine animals from coastal areas of Zhejiang were analyzed and evaluated for the purpose of further understanding the situations of pollution level in this area. The results are listed as follows.
An isotope dilution-high resolution gas chromatography/ion trap mass Spectrometry (HRGC/ITMS) method with purification-separation by gel permeation chromatography (GPC) and aluminosilicate column techniques was developed for quantification and identification of 20 organochlorine pesticides (OCPs), 28 PCB congeners and 16 PAH compounds in marine shellfishes. The GPC elution time for target chemicals and elution volumes of two continual eluting solvents from aluminosilicate column were optimized. The results showed that the method detection limits were 0.01～0.14 for PCBs, 0.02～0.17 for OC pesticides and 0.52～0.81 ng/g (wet weight) for PAHs. The recovery percentages and RSDs of two-level spiked samples were in the ranges of 84.1%～120.2% and 5.6～15.9% for PCBs, 62.3%～123.1% and 8.7～20.5% for PAHs, and 77.3%～127.5% and 3.1～18.7% for OC pesticides, respectively. In this method, three groups of organic compounds from shellfishes were simultaneously cleaned up and separated. The method reduced cost and time for sample pretreatment and was applied in analyzing POPs in marine organisms of the study.
By using the established HRGC/ITMS method for analyzing multiresidual POPs in marine organisms, the levels of OC pesticides, PCBs and PAHs in shellfishes, fishes and shrimps collected from 12 counties (cities) from coastal areas of Zhejiang were analyzed and the results were summarized as follows.
The predominating components of organochlorine (OC) pesticides in marine organisms were p,p'-DDE, p,p'-DDD, p,p'-DDT,γ-chlordan andα-chlordan. The ratios of DDT/(DDE+DDD) indicated that DDTs pesticides or input of new pesticides containing DDTs pesticides possibly existed in six areas such as Shengsi, Putuo, Ninghai, Yueqing, Jiaojiang and Yuhuan.
In this study, PCB52、PCB66、PCB153、PCB138、PCB101、PCB180 and PCB118 were the predominating congeners in examined shellfishes, Bombay duck (Harpodon nehereus) and Exopalaemen carinicauda. The hexa-chlorinated PCB congeners in marine organisms were predominant followed by tetra, penta, tri and hepta chlorinated PCB congeners.
The PAHs compounds in shellfishes were dominated by highly condensed ring structure while the two and three-ring PAHs in Bombay duck and Exopalaemen carinicauda were the predominating compounds..
The levels of POPs in shellfishes were markedly higher than those in Bombay duck and Exopalaemen carinicauda indicating the stronger abilities of shellfishes in accumulating POPs. The distribution features of POPs in marine organisms from the study area showed that the levels of PCBs and PAHs in shellfishes from Yueqing were higher, while OC pesticides and PAHs in shellfishes from Shengsi and Putuo were in higher levels. The levels of OC pesticides and PAHs in Bombay duck from the study area were in similar levels except that PCBs in Bombay duck from Jiaojiang was in higher level. The levels of OC pesticides and PCBs in Exopalaemen carinicauda from Ninghai and Yuhuan were higher, while PAHs in the study area were in similar levels.
The levels of DDTs in some samples of shellfishes, Bombay duck and Exopalaemen carinicauda had exceeded the tolerance levels of Europe, USEPA and marine organisms quality standards of China. Among them, the shellfishes had the highest ratios of exceeding tolerance. The results of cancer risks evaluation indicated that the EDI values of organic pollutants in marine organisms were lower than the corresponding values of RfD and CBC. Furthermore, the EDI values of DDTs and HCHs were much lower than the ADI values recommended by FAO/WHO. There are no cancer risks existed for the residents of Zhejiang province in consuming fishery products such as shellfishes, Bombay duck and Exopalaemen carinicauda.
The results of organic pollutants in surface sediments from Changjiang estuary, Hangzhou Bay and Zhoushan marine area showed that the area with the higher values of organic pollutants was found in Nanhuizui area near the south branch of Changjiang estuary and north bank of Hangzhou Bay. The levels of organic pollutants in sediments from north branch of Changjiang estuary were significantly lower than those from south branch indicating that the organic pollutants were mainly from land based sources, especially from runoffs of Changjiang River.
The predominant distribution patterns of PAHs in the surface sediments, grouped by number of rings, were the same in the study area. PAHs in sediments were dominated by 3- and 4-ring followed by 5-, 2- and 6-ring PAHs. The sources of PAHs were mainly from pyrogenic or combustion of wood and coal, the petroleum pollution was also one of sources of PAHs in sediments. PCBs in sediments were dominated by low chlorinated PCB congeners. The ratios of DDT/(DDE+DDD) indicated that no new input sources of DDTs pesticides existed in the study area.
The results showed that organic carbon contents was a dominating factor controlling the levels of PAHs, PCBs and OC pesticides in sediments and the organic pollutants had the same characteristics of source, i.e. runoffs of Changjiang River.
The levels of PAHs, PCBs and OC pesticides in most sediment samples were lower than the corresponding ER-L values of NOAA SQG, indicating that overall quality status of sediments was in good conditions. However, fluorene concentrations in some sampling sites near south branch of Changjiang estuary and mouth of Hangzhou Bay exceeded the ER-L value, while DDTs levels in sediments of over half sampling sites exceeded the ER-L value. The overall concentrations of organic pollutants in the study area were in lower or medium level compared with those from other areas.
In the study area, the surface sediments analyzed by grain size were mainly composed of clayey silt and silt. The total levels of Cu, Cr, Fe and Ni in surface sediments were lower than the background contents, while Pb, Zn and Mn concentrations were higher than the background values in the middle of Hangzhou Bay and inner Yangtze River estuary. The distribution of total metal concentrations in the study area showed similar patterns, decreasing from the inner toward the mouth of Yangtze River estuary or Hangzhou Bay. However, elevated levels of heavy metals were observed in the middle of Hangzhou Bay. The total concentrations of heavy metals were lower than the Grade II of Marine Sediment Quality of China or ER-M and PEL values. Further correlation analyses confirmed that the levels of heavy metals and organic carbon were highly correlated with the clay component of the surface sediments, indicating that the variations of heavy metals and organic carbon concentrations were controlled by grain size of the terrigenous sediments. The high positive correlations among heavy metals showed that the surface sediments were from a similar terrigenous source or a result of similar mechanisms of transport and accumulation within the sediments. Sequential extraction analyses indicated that the heavy metals (Cr, Fe, Ni, Pb, Zn and Cu) were mainly retained in the residual fraction, suggesting lower pollution risks with respect to those metals, while Cd and Mn had the potential risks of environmental pollution.
Cu, Pb, Zn, Cd, Hg and As in fishes, shellfishes, shrimps and cephalopods from coastal areas of Zhejiang were in lower levels compared with those from domestic and foreign countries. The levels of Zn and Cu in marine organisms were relatively higher, while those of Pb、Cd、As and Hg were in lower levels. The shellfishes had strongest abilities in accumulating heavy metals followed by cephalopods, shrimps and fishes. The results of evaluation indicated that the examined marine organisms were not heavily contaminated by heavy metals, while Cu and Cd in shellfishes, As and Zn in fishes and As in shrimps were in minor pollution level. Except that Cd in shellfishes and shrimps, and As in shrimps exceeded the tolerance levels of Australian standard, other heavy metals were inferior to the tolerance levels suggesting that the overall quality status of marine organisms in the study area was in good condition.
1．建立了同时对海洋贝类中20种有机氯农药、28种多氯联苯和16种多环芳烃的同位素稀释气相色谱—离子阱质谱分析方法，确定了凝胶净化色谱的最佳组分收集时间和铝硅胶柱两种连续淋洗溶剂的体积。结果表明，多氯联苯、有机氯农药和多环芳烃各化合物的方法检出限分别为0.01-0.14，0.02～0.17和0.52～0.81 ng/g(湿重)，样品的加标回收率和相对标准偏差分别为：多氯联苯84.1％～120.2％，5.6～15.9％；多环芳烃62.3％～123.1％，8.7～20.5％；有机氯农药77.3％～127.5％，3.1～18.7％。
2．以所建立的分析方法对采自浙江沿海12个县(市)的贝类、鱼类和虾类等生物样品进行了有机氯农药、多氯联苯和多环芳烃含量的分析，结果表明：
生物体内有机氯农药的主要化合物是p，p′-DDE，p，p′-DDD，p，p′-DDT，γ-氯丹和α-氯丹。DDT／(DDE+DDD)比值判断结果表明：嵊泗、普陀、宁海、乐清、椒江和玉环等六个区域可能存在着DDT类农药或含DDT的农药新的来源。贝类中的多氯联苯以六氯代同族体为主要组成，其次分别为四氯代、五氯代、三氯代和七氯代。贝类中多环芳烃以高苯环数的为主，而龙头鱼和脊尾白虾体内的多环芳烃主要以低苯环数的二环和三环为主。
从生物种类来看，贝类体内多氯联苯、多环芳烃和有机氯农药水平明显高于龙头鱼和脊尾白虾，反映贝类对有机污染物具有较强的积蓄能力。区域分布特征表明，乐清贝类体内的多氯联苯和多环芳烃的含量较高，而嵊泗和普陀贝类有机氯农药和多环芳烃处于较高水平。除椒江龙头鱼多氯联苯含量较高外，各区域龙头鱼中有机氯农药和多环芳烃含量接近。宁海和玉环脊尾白虾有机氯和多氯联苯的含量较高，各区域脊尾白虾中的多环芳烃含量接近。
贝类、龙头鱼和脊尾白虾部分样品的DDTs超过欧盟、美国EPA和我国海洋生物标准的限值，其中贝类的超限值率为最高。致癌风险评价结果表明：生物体内有机污染物的EDI值均低于相对应的RfD和CBC值。生物体内的DDTs和HCHs的EDI值也远低于FAO／WHO推荐的ADI(可接受每日摄入量)。对浙江居民来说，目前食用贝类、龙头鱼和脊尾白虾不会对其构成致癌风险。
3．研究区域表层沉积物中多环芳烃、多氯联苯和有机氯农药这三类有机污染物的高值区均出现在长江口南支南汇嘴附近和杭州湾北岸。长江口北支口外海域沉积物中的含量明显低于南支附近海域。沉积物中有机污染物主要是受陆域污染源，特别是长江径流的影响。
长江口、杭州湾和舟山海区表层沉积物多环芳烃的组成规律相同，均为三环＞四环＞五环＞二环＞六环。多环芳烃主要来源于油类与木柴、煤的燃烧，而石油产品的泄漏排放也是其来源之一。沉积物中多氯联苯主要是以低氯代的多氯联苯同族体为主。而沉积物的DDT／(DDE+DDD)比值显示研究区域总体上没有DDT类农药新的输入来源。
沉积物中的有机碳是影响多环芳烃、多氯联苯和有机氯农药含量的主要因素。表层沉积物中多环芳烃、多氯联苯和有机氯农药具有长江径流来源的这一相同特征。
多环芳烃、有机氯农药和多氯联苯组分含量大部分低于美国NOAASQG的ER-L值，沉积物质量状况总体上处于良好的状态。长江口南支附近和杭州湾湾口部分沉积物中的芴浓度和半数以上站位DDTs含量已超过了ER-L值。研究区域沉积物中的多环芳烃、多氯联苯和有机氯农药(HCHs和DDTs)的含量总体上处于较低或中等水平。
4．研究区域中，表层沉积物主要组成类型为粉砂和粘土质粉砂。沉积物中的Cu、Cd、Cr、Fe和Ni的总量低于背景值；而杭州湾中部和长江口口内沉积物Pb、Zn和Mn高于背景值。在长江口区域，沉积物中重金属含量从长江口南支内向口外方向递减；杭州湾沉积物重金属亦有湾内向湾外方向降低的趋势，但湾中部沉积物重金属含量较高。沉积物中的重金属均未超出沉积物二类控制标准或ER-M、PEL值。陆源沉积物的颗粒粒径是影响沉积物重金属和有机碳水平的重要因素。研究区域沉积物可能具有相同来源或相似的输送和积累机理。沉积物中的Cr、Fe、Ni、Pb、Zn和Cu主要存在于残留态中，对环境污染的风险较低，而沉积物中的重金属Cd和Mn具有潜在的环境污染风险。
5．与国内外沿海区域相比较，浙江沿岸海域鱼类、贝类、虾类和头足类体内Cu、Pb、Zn、Cd、Hg和As的含量水平总体上处于较低的水平。其中，Zn和Cu元素的含量为最高，而其它重金属Pb、Cd、As和Hg含量相对较低。贝类对重金属元素的积累能力为最强，头足类次之，其次为虾类，而积累能力最弱的为鱼类。所研究的海洋生物未受到重金属的严重污染，但贝类的Cu和Cd，鱼类的As和Zn，以及虾类的As处于轻度污染水平。除贝类和虾类的重金属Cd和虾类的As含量超出了澳大利亚的“人体消费卫生标准”的限值外，其它重金属含量均低于食用限值，表明研究区域的海洋生物质量总体上处于良好的状态。
Zhejiang province is located in the southeast coastal areas of China, with the total coastline about 6,321 km in length. There are four bays, i.e. Hangzhou bay, Xiangshan harbour, Sanmen bay and Yueqing bay, and 3,016 islands in this area. The region also includes Zhoushan fishing ground, which is the largest one in China and an internationally important fishing ground that contains many actual and potential maricultural sites. In recent twenty years, with the rapid economic development of Changjiang Delta area, the coastal environment was increasingly influenced by pollutants from Changjiang River and Qiangtang River runoffs, and non-point land-based pollutants from Jiangsu, Zhejiang and Shanghai in addition to activities of marine aquaculture, fishing and shipping, etc. The status of environmental quality in the area is deteriorating in recent years. In this study, the levels, distribution features, impact factors and ecological risks of the persistent organic pollutants (POPs), i.e. polychlorinated biphenyls, polycyclic aromatic hydrocarbons and organochlorine pesticides, and heavy metals in surface sediments from Changjiang estuary, Hangzhou Bay and Zhoushan marine areas and marine animals from coastal areas of Zhejiang were analyzed and evaluated for the purpose of further understanding the situations of pollution level in this area. The results are listed as follows.
An isotope dilution-high resolution gas chromatography/ion trap mass Spectrometry (HRGC/ITMS) method with purification-separation by gel permeation chromatography (GPC) and aluminosilicate column techniques was developed for quantification and identification of 20 organochlorine pesticides (OCPs), 28 PCB congeners and 16 PAH compounds in marine shellfishes. The GPC elution time for target chemicals and elution volumes of two continual eluting solvents from aluminosilicate column were optimized. The results showed that the method detection limits were 0.01～0.14 for PCBs, 0.02～0.17 for OC pesticides and 0.52～0.81 ng/g (wet weight) for PAHs. The recovery percentages and RSDs of two-level spiked samples were in the ranges of 84.1%～120.2% and 5.6～15.9% for PCBs, 62.3%～123.1% and 8.7～20.5% for PAHs, and 77.3%～127.5% and 3.1～18.7% for OC pesticides, respectively. In this method, three groups of organic compounds from shellfishes were simultaneously cleaned up and separated. The method reduced cost and time for sample pretreatment and was applied in analyzing POPs in marine organisms of the study.
By using the established HRGC/ITMS method for analyzing multiresidual POPs in marine organisms, the levels of OC pesticides, PCBs and PAHs in shellfishes, fishes and shrimps collected from 12 counties (cities) from coastal areas of Zhejiang were analyzed and the results were summarized as follows.
The predominating components of organochlorine (OC) pesticides in marine organisms were p,p'-DDE, p,p'-DDD, p,p'-DDT,γ-chlordan andα-chlordan. The ratios of DDT/(DDE+DDD) indicated that DDTs pesticides or input of new pesticides containing DDTs pesticides possibly existed in six areas such as Shengsi, Putuo, Ninghai, Yueqing, Jiaojiang and Yuhuan.
In this study, PCB52、PCB66、PCB153、PCB138、PCB101、PCB180 and PCB118 were the predominating congeners in examined shellfishes, Bombay duck (Harpodon nehereus) and Exopalaemen carinicauda. The hexa-chlorinated PCB congeners in marine organisms were predominant followed by tetra, penta, tri and hepta chlorinated PCB congeners.
The PAHs compounds in shellfishes were dominated by highly condensed ring structure while the two and three-ring PAHs in Bombay duck and Exopalaemen carinicauda were the predominating compounds..
The levels of POPs in shellfishes were markedly higher than those in Bombay duck and Exopalaemen carinicauda indicating the stronger abilities of shellfishes in accumulating POPs. The distribution features of POPs in marine organisms from the study area showed that the levels of PCBs and PAHs in shellfishes from Yueqing were higher, while OC pesticides and PAHs in shellfishes from Shengsi and Putuo were in higher levels. The levels of OC pesticides and PAHs in Bombay duck from the study area were in similar levels except that PCBs in Bombay duck from Jiaojiang was in higher level. The levels of OC pesticides and PCBs in Exopalaemen carinicauda from Ninghai and Yuhuan were higher, while PAHs in the study area were in similar levels.
The levels of DDTs in some samples of shellfishes, Bombay duck and Exopalaemen carinicauda had exceeded the tolerance levels of Europe, USEPA and marine organisms quality standards of China. Among them, the shellfishes had the highest ratios of exceeding tolerance. The results of cancer risks evaluation indicated that the EDI values of organic pollutants in marine organisms were lower than the corresponding values of RfD and CBC. Furthermore, the EDI values of DDTs and HCHs were much lower than the ADI values recommended by FAO/WHO. There are no cancer risks existed for the residents of Zhejiang province in consuming fishery products such as shellfishes, Bombay duck and Exopalaemen carinicauda.
The results of organic pollutants in surface sediments from Changjiang estuary, Hangzhou Bay and Zhoushan marine area showed that the area with the higher values of organic pollutants was found in Nanhuizui area near the south branch of Changjiang estuary and north bank of Hangzhou Bay. The levels of organic pollutants in sediments from north branch of Changjiang estuary were significantly lower than those from south branch indicating that the organic pollutants were mainly from land based sources, especially from runoffs of Changjiang River.
The predominant distribution patterns of PAHs in the surface sediments, grouped by number of rings, were the same in the study area. PAHs in sediments were dominated by 3- and 4-ring followed by 5-, 2- and 6-ring PAHs. The sources of PAHs were mainly from pyrogenic or combustion of wood and coal, the petroleum pollution was also one of sources of PAHs in sediments. PCBs in sediments were dominated by low chlorinated PCB congeners. The ratios of DDT/(DDE+DDD) indicated that no new input sources of DDTs pesticides existed in the study area.
The results showed that organic carbon contents was a dominating factor controlling the levels of PAHs, PCBs and OC pesticides in sediments and the organic pollutants had the same characteristics of source, i.e. runoffs of Changjiang River.
The levels of PAHs, PCBs and OC pesticides in most sediment samples were lower than the corresponding ER-L values of NOAA SQG, indicating that overall quality status of sediments was in good conditions. However, fluorene concentrations in some sampling sites near south branch of Changjiang estuary and mouth of Hangzhou Bay exceeded the ER-L value, while DDTs levels in sediments of over half sampling sites exceeded the ER-L value. The overall concentrations of organic pollutants in the study area were in lower or medium level compared with those from other areas.
In the study area, the surface sediments analyzed by grain size were mainly composed of clayey silt and silt. The total levels of Cu, Cr, Fe and Ni in surface sediments were lower than the background contents, while Pb, Zn and Mn concentrations were higher than the background values in the middle of Hangzhou Bay and inner Yangtze River estuary. The distribution of total metal concentrations in the study area showed similar patterns, decreasing from the inner toward the mouth of Yangtze River estuary or Hangzhou Bay. However, elevated levels of heavy metals were observed in the middle of Hangzhou Bay. The total concentrations of heavy metals were lower than the Grade II of Marine Sediment Quality of China or ER-M and PEL values. Further correlation analyses confirmed that the levels of heavy metals and organic carbon were highly correlated with the clay component of the surface sediments, indicating that the variations of heavy metals and organic carbon concentrations were controlled by grain size of the terrigenous sediments. The high positive correlations among heavy metals showed that the surface sediments were from a similar terrigenous source or a result of similar mechanisms of transport and accumulation within the sediments. Sequential extraction analyses indicated that the heavy metals (Cr, Fe, Ni, Pb, Zn and Cu) were mainly retained in the residual fraction, suggesting lower pollution risks with respect to those metals, while Cd and Mn had the potential risks of environmental pollution.
Cu, Pb, Zn, Cd, Hg and As in fishes, shellfishes, shrimps and cephalopods from coastal areas of Zhejiang were in lower levels compared with those from domestic and foreign countries. The levels of Zn and Cu in marine organisms were relatively higher, while those of Pb、Cd、As and Hg were in lower levels. The shellfishes had strongest abilities in accumulating heavy metals followed by cephalopods, shrimps and fishes. The results of evaluation indicated that the examined marine organisms were not heavily contaminated by heavy metals, while Cu and Cd in shellfishes, As and Zn in fishes and As in shrimps were in minor pollution level. Except that Cd in shellfishes and shrimps, and As in shrimps exceeded the tolerance levels of Australian standard, other heavy metals were inferior to the tolerance levels suggesting that the overall quality status of marine organisms in the study area was in good condition.
引文
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