温瑞塘河中持久性有毒物质的污染特征与源解析
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摘要
随着社会经济发展,人类生产生活与自然过程产生的污染物越来越多,组成也越来越复杂,一些具有持久性,生物毒性的痕量污染物对水环境形成危害。持久性有毒物质是一类具有很强生物毒性与生态毒性,在环境中难以降解,并通过食物链在生态系统中不断积累、富集和放大的痕量污染物。在地球空间的固、气、液进行循环并可通过长距离大尺度的迁移,进入水环境中,可直接通过上覆水作用于生物体,也可在水体物化与生物作用下在上覆水-间隙水-沉积物之间迁移转化,对水环境质量形成持久性的影响,进一步影响到水生生态系统安全。水环境中持久性有机污染物,重金属类污染物属环境中典型的污染物,对人类与自然环境危害大,影响深远,其自然修复难度大,人工措施去除成木高且方法不成熟,受到国内外学者高度关注。
温瑞塘河是温州市最大的城市河网,被温州人民称为“母亲河”。温州市中小企业及家庭作坊式生产十分发达,在生产过程中由于管理松散而导致的污染物无序排放,进入水环境形成污染。本研究在国家重大水专项课(2009ZX07317-006);国家自然基金委青年科学基金(41101471)支助下,以温瑞塘河为研究对象,通过对上覆水、间隙水、沉积物中持久性有毒物质检测分析,利用发光细菌与热带爪蟾胚胎表征水环境生物毒性,利用数理统计分析方法解析持久性有毒物质的污染来源。揭示温瑞塘河水环境中持久性有毒物质(Cd、Cr、Pb、Hg、As、Cu、 Zn、Ni、PAHs)的空间分布特征、污染来源,水环境生物毒性及在模式生物的表现,水环境受污染程度与生态风险,为温瑞塘河水环境污染治理、水资源可持续利用与管理提供理论参考。本研究主要得到以下结论：
(1)在温瑞塘河上覆水与间隙水中重金属元素含量平均值大于地表水V标准,表明河流受到重金属污染,上覆水中Cd、Hg、Cr、Mn、Ni、Cu重金属元素含量低于间隙水,Zn元素例外,部分采样点上覆水中重金属含量高于间隙水,表明部分区域仍存在高浓度重金属污染。在温瑞塘河沉积物中各重金属元素的区间值(mg/kg)Hg(0.18～7.31)、Cd(0～149.53)、Cr(43.9～1892.70)、Pb(17.31～162.93)、As(2.12-17.79)、Cu(19.23-3393.81)、Zn(119.27-4934.87)、Ni(16.72～1646.09)。重金属Cd、Zn元素含量最高点位于温瑞塘河主干河道城市与工业集中区及支流河道的汇流区,其次为冶炼、电镀小企业集中的三垟湿地人口聚集区,支流源头区、农业及城市远郊区低。柱状样重金属垂直分布特征显示,重金属污染受农业污染源的影响在减轻,但农业面源污染仍存在,工业污染源、生活污染源污染呈增长趋势。Cd、Cr、Pb、Cu、Zn、Ni、Fe重金属元素形态为残渣态高于其他形态,可被生物利用有效态为Cd(66.75%)>Mn(65.90%)>Ni(63.55%)>Cu(60.24%)>Pb(59.67%)>Zn(58.61%)>Cr(54.70%)>Fe(23.69%)。
(2)沉积物单一重金属元素污染指数(Cfi)的评价结果为Cd(76.92)>Cu(17.4)>Hg(10.66)>Zn(9.19)>Ni(5.69)>Cr(4.30)>As(1.46)>Pb(1.43)。综合污染指数(Cd)评价受到重金属严重污染的采样点达14个,受重污染采样点为7个中污染采样点为8个,严重污染的采样点中Cd、Cu、Hg、Zn、Ni元素属严重污染状态。重金属的潜在生态危害指数(Eri)评价值为Cd(2307.47)>Hg(426.25)>Cu(87.03)>Ni(28.45)>As(14.58)>Zn(9.19)>Cr(8.60)>Pb(7.14)。重金属的生态风险指数RI结果显示采样点达极强生态风险点17个,强生态风险点7个,其中8##点生态风险最强,25#点生态风险最低点,河道沉积物受重金属Hg、Cd的污染存在很强的潜在生态风险可能。
(3)沉积物中重金属元素平均富集指数顺序为Cd(126.7)>Cu(33.1)>Zn(16.3)>Hg(14.71)>Ni(10.7)>Cr(7.80)>As(2.63)>Pb(2.6),其中As、Pb元素属于中污染,Cr、Ni、Hg、Zn属于偏重污染,Cu属于重污染,Cd属于严重污染。整个河道沉积物受Cd、Hg污染采样点区域最多,处于偏重污染程度的采样点百分比>75.86%,重金属元素As、Pb对沉积物污染最轻,其处于偏重污染程度的采样点百分比<6.90%。在内梅罗污染指数基础上建立的综合地累积指数评价表明沉积物受到Hg、Cd、Cu、Zn,Ni和Cr污染,采样点区域污染程度依次为机械工业园区>主河道城市区>三垟湿地区>城市周边区>水源地区。
(4)温瑞塘河的重金属污染主要来自于人为活动的影响,其重金属人为贡献率为Hg(86.62%)>Cd(81.20%)>Zn(80.59%)>Cu(75.86%)>Ni(68.12%)>Cr(64.26%)>As(54.7%)>Pb(45.78%),相关性分析与主成分分析表明Hg、Cd、Cu、Zn、Ni和Cr具有极显著相关性,来源以人为源为主,但也受到地球化学组成影响。
(5)多环芳烃在上覆水样中的含量Mean=128.13ng.L-1、Min=28.91ng.L-1、 Max=440.04ng.L-1,结构主要由低环(2+3)组成,PAHs含量机械工业园区域,城市生活与工厂混杂区域,城市生活旧城区域的含量较高。间隙水样的PAHs含量为Mean=631.87ng.L-1、Min=57.56ng.L-1、Max=1628.50ng.L-1,平均值大于上覆水样,结构以低环(2+3)为主。沉积物中PAHs含量Mean=1314.58ng.g-1、 Min=152.85ng.g-1、Max=3826.80ng.g-1,PAHs单体主要由2-6环组成,低环(2+3)结构平均占37.37%,中环(4)结构平均占37.41%,高环(5+6)结构平均占25.22%。PAHs在沉积物中的含量顺序为机械工业园区、城市生活与工厂混杂区、城市生活旧城区、支流河道交汇区、干流区与源头区。沉积物分层柱状样的PAHs含量在1#、3#、10#、14#、18#、20#点第一层高于第二和第三层,表明其污染日前处于加重趋势,2#、4#、7#、15#、16#、19#、21#、23#点第一层低于第二层或第三层,表明污染在降低。
(6)温瑞塘河上覆水水样的TEQ值范围在0.02-16.15ng.L-’,平均值2.62ng.L-1,平均值低于地表水质环境标准的2.8ng'L-1,毒性当量处于安全防范之内,在采样点中高于水质标准点7个,这些点具有较高生态风险。水环境中最小风险值范围15.42～1684.28,平均值为315.06,最大风险值范围0.15-16.84,平均值3.15,属高风险等级点4个,属中等风险等级点17个点,属低风险等级8个点沉积物中PAHs单体浓度值没有点超过生态效应值ERM,PAHs单体易发生生态风险的可能性小。沉积物毒性当量法的生物毒性区间(9.49-1331.09ng.g-1)平均值为158.2ng.g-1,沉积物最小风险商值平均值为438.99,风险商值区间为55.36～2833.31,属中等风险及以上样点达82.8%,具有发生潜在生态风险的可能。
(7)聚类分析与主成分分析表明温瑞塘河水样中PAHs单体的中高环由发热源产生,2-3环低分子量或者烷基取代类PAHs来自自然源或石油泄漏等。由FIu/(Flu+Pyr), Ant/(Ant+Phe)比值表明多环芳烃主要来源为燃烧来源,其中石油燃烧源占23.1%,其余为薪材等燃烧热源为76.9%,由FIu/(Flu+Pyr), BaA/(BaA+Chr)比值分析采样点PAHs来源,石油燃烧源4个,石油、薪材、煤混合源6个,高温薪材燃烧源12个。利用聚类分析表明温瑞塘河沉积物的PAHs来源中高环单体主要是发热源产生,2-3环低分子量或者烷基取代类PAHs主要来自自然源-石油泄露等,由主成分分析沉积物中PAHs污染来源,主成分分析与柴油车和天然气、汽油燃烧排放相关,该主成分可视为交通和与交通相关的污染来源,存在薪材类燃烧与石油相关产品挥发或泄漏源。由Ant/(Ant+Phe)特征比值显示有6个点为石油类污染源,FIu/(FIu+Pyr)比值显示薪材类燃烧源占75.8%,也存在石油燃烧与石油泄漏源。由FIu/(FIu+Pyr), BaA/(BaA+Chr)比值可知,主要由薪材类物质的燃烧的源点占82.8%,石油类物质的燃烧与泄漏混合源占17.2%。由FIu/(Flu+Pyr), Inp/(Inp+BghiP)特征值可知,55%的点为薪材燃烧源,其余为石油泄漏源。
(8)利用青海弧菌(Q7)对温瑞塘河上覆水,间隙水,沉积物生物毒性研究结果为上覆水样的平均发光强度为80.9%,属轻微毒性,间隙水相对发光强度的平均值69.7%,属中等生物毒性,沉积物相对发光强度的平均值63.3%,属中等生物毒性,上覆水相对发光强度>间隙水相对发光强度>沉积物的相对发光强度。沉积物浸出液对热带爪蟾胚胎发育毒性结果平均孵化率为75.98%,平均成活率为83.77%,平均致畸率为16.60%,平均体长为3.58cm。采样点污染源复杂与污染严重采样点对爪蟾胚胎发育生长毒性大,河流源头区及污染源单一采样点生物毒性小。
With the social and economic development, more and more pollutants with complex components are produced by human activity and natural process. Some trace pollutants which are persistent and biotoxic pose serious threat to the aquatic environmental. Persistent toxic substances are contaminants of strong biotoxicity and ecotoxicity, which are difficult to be degraded in the environment and constantly accumulate, enrich and magnify through the food chain in the ecosystem. Persistent toxic substances (PTS) can transport long distance in large scale via solid, gas and liquid. When PTS enter aquantic environment, they can affect living organisms directly through the overlying water, and also transport and transform among the overlying water-gap water-sediment through physical, chemical and biological processes of the water bodies. Thus, PTS have lasting impacts on the quality of the aquantic environment and furtherly affect the safety of the aquatic ecosystem. The persistent organic pollutants and heavy metal contaminant, two kinds of typical PTS in the aquatic environment, are hazardous to human beings and the nature since their impacts could be far-reaching and significant and their remediation is either hard and slow by nature process or costly and imperfect by artificial measures. Therefore, PTS in aquatic environment have been highly concerned worldwide.
Wenruitang River, the "mother river" called by the local people, is the largest urban river network in Wenzhou City. Wenzhou is famous for its small-medium sized enterprises and family workshops, pollutants are disorderly discharged to the aquatic environment in the production process due to the loose environmental management. With the support of the National Major Project (2009ZX07317-006) and the National Natural Science Youth Foundation of China (41101471), this dissertation took Wenruitang River as the research object, investigated the PTS in the surface water, pore water and sediments from Wenruitang River by chemical analysis, determined the PTS pollution sources through statistical analysis, assessed the biological toxicity of the PTS via light-emitting bacteria and tropical Xenopus embryos. It revealed the spatial distribution characteristics of PTS (Cd, Cr, Pb, Hg, As, Cu, Zn, Ni and PAHs) in Wenruitang River, pollution sources, PTS biological toxicity and the response of model organisms to PTS, assessed the contamination degree and ecological risk of PTS in Wenruitang River, hopefully to provide a theoretical reference for river pollution treatment and the sustainable use and management of river water resources. The major conclusions of this research are listed as follows:
(1) The average heavy metal content in the surface water and pore water from Wenruitang River was higher than the corresponding value in the level V of the surface water standard of China, which showed that the river was polluted by heavy metals. The content of Cd, Hg, Cr, Mn, Ni and Cu in the surface water was less than that in the pore water. Zn was an exception, for its concentration in the surface water from some of the sampling sites was higher than that in the pore water from the same place. The interval values (mg/kg) of heavy metals from the sediments of Wenruitang River were:Hg (0.18～7.31), Cd (0～149.53), Cr (43.9～1892.70), Pb (17.31～162.93), As (2.12～17.79), Cu (19.23～3393.81), Zn (119.27～4934.87) and Ni (16.72～1646.09). The sampling site with the maximum Cd and Zn contents located in the main channel of Wenruitang River where residential area and industrial area were overlapped, following by Sanyang wetland area where small smelting and plating factories used to concentrated there, and the minimum Cd and Zn contents in agriculture and exurban area. Vertical distribution characteristics of heavy metal in core sediment samples showed that heavy metal pollution caused by agricultural sources was reduced while pollution caused by industrial sources and residential sources were increasing. Heavy metals Cd, Cr, Pb, Cu, Zn, Ni and Fe were mostly in the form of residual fraction rather than other forms. The bioavailable state of these heavy metals were Cd (66.75%)> Mn (65.90%)> Ni (63.55%)> Cu (60.24%)> Pb (59.67%)> Zn (58.61%)> Cr (54.70%)> Fe (23.69%).
(2) The evaluation result of the sediment single element pollution index (Cf1) was Cd (76.92)> Cu (17.4)> Hg (10.66)> Zn (9.19)> Ni (5.69)> Cr (4.30)> As (1.46)> Pb (1.43). The evaluation results of integrated Pollution Index (Cd) indicated that the numer of seriously, heavily and moderately polluted sampling sites was14,7and8, respectively. Among the seriously polluted sampling sites, Cd, Cu, Hg, Zn, and Ni belonged to the serious pollution level. The order of potential ecological risk index (Er1) was Cd (2307.47)> Hg (426.25)> Cu (87.03)> Ni (28.45)> As (14.58)> Zn (9.19)> Cr (8.60)> Pb (7.14). The results of the ecological risk index RI showed that there were17sampling sites of extremely strong ecological risk,7sampling sites of strong ecological risk and no site of low ecological risk. The highest ecological risk appeared at sampling site8#while the lowest was at sampling site25#. Hg and Cd had strong potential ecological risk.
(3) The order of the average enrichment index of heavy metals in the sediment was Cd (126.7)> Cu (33.1)> Zn (16.3)> Hg (14.71)> Ni (10.7)> Cr (7.80)> As (2.63)> Pb (2.6). According to this order, As and Pb belonged to moderate pollution, Cr, Ni, Hg and Zn belonged to moderate to heavy pollution, Cu belonged to heavy pollution, Cd belonged to serious pollution. The entire river sediments were mostly polluted by Cd and Hg in term of polluted area with more than75.86%sampling sites were no less than the level of moderately to heavily contaminated, whereas As and Pb were leastly polluted with less than6.90%sampling sites were in the level of more serious pollution. Based on the Nemerow Pollution Index, a comprehensive geoaccumulation index was established. The geoaccumulation index showed that the sediments were polluted by Hg, Cd, Cu, Zn, Ni and Cr. The pollution level order of different region was machinery industrial park> main river city downton section> Sanyang Wetland> suburban areas> drinking water source areas.
(4) Heavy metal pollution in Wenruitang River mainly affected by human activities. The anthropogenic contribution rate of each heavy metal was Hg (86.62%)> Cd (81.20%)> Zn (80.59%)> Cu (75.86%)> Ni (68.12%)> Cr (64.26%)> As (54.7%)> Pb (45.78%). The correlation analysis and principal component analysis indicated that Hg, Cd, Cu, Zn, Ni and Cr were significantly correlated. Heavy metals in Wenruitang River were mainly originated from anthropogenic sources, and affected by geochemical process at the mean time.
(5) The minimum, maximum and mean concentration of polycyclic aromatic hydrocarbons in the surface river water was28.91ng.L-1,440.04ng.L-1and128.13ng.L-1, respectively. PAHs structure composed mainly by low ring (2+3). PAHs had higher concentration in machinery industrial park area, residential and industrial mixed area as well as the old city area. The maximum, mean and minimum concentrations of PAHs in interstitial water were1628.50ng.L-1,631.87ng.L-1and57.56ng.L-1, respectively. The average PAHs concentration in the interstitial water was greater than that in the surface water samples. The PAHs structure composed mainly by the low ring (2+3). The minimum, maximum and mean contents of PAHs in the sediments were152.85ng.g-1,3826.80ng.g-1and1314.58ng.g-1, respectively. PAHs monomer mainly composed by2～6rings, low ring (2+3) structure accounted for37.37%by average, middle ring (4) structure accounted for37.41%, high ring (5+6) structure accounted for25.22%. The order of PAHs content in sediments were machinery industrial park area> residential and industrial mixed area> the old city area> tributary confluence area> the main river stream and the river source area.
The PAHs content in the sediment column sample showed that the first layer had higher PAHs than the second and third layers from samples1#,3#,10#,14#,18#and20#, which revealed that the pollution was aggravating. PAHs content in the first layer was lower than that in the second and third layers from samples2#,4#,7#,15#,16#,19#,21#and23#, which indicated that the pollution was reducing.
(6) The TEQ values of surface water samples of Wenruitang River ranged from0.02to16.15ng.L-1. The average value was2.62ng.L-1, which is lower than2.8ng.L-1defined by the surface water quality environmental standards, meaning that the toxic equivalence was in security. There were7sampling sites with TEQ value higher than the surface water quality standards. These sampling sites would face higher ecological risk. The minimum risk value ranged from15.42to1684.28with the average value of315.06. The maximum risk value ranged from0.15to16.84with the average of3.15. There were4high-risk rating sties,17medium risk rating sites and8low risk rating sites. PAHs monomer concentration in sediments exceeding the ecological effects ERM was not found, so PAHs monomer in sediments was not liketly to induce ecological risk. The average biological toxicity by sediment toxicity equivalent methodwas158.2ng.g-1(ranged from9.49to1331.09ng.g-1). The average sediment minimum risk quotient is438.99, the risk quotient value ranged from55.36to2833.31. The samples had at least medium risk accounted for82.8%, indicating the possibility of potential ecological risk.
(7) The cluster analysis and principal component analysis demonstrated that middle and high ring of PAHs monomer was generated by the heat source, the low ring with low molecular weight or alkyl substituted class of PAHs was originated from natural sources or oil spill. The FIu/(Flu+Pyr), Ant/(Ant+Phe) ratios indicated that the main source of polycyclic aromatic hydrocarbons was combustion sources, including23.1%oil combustion sources and76.9%fuelwood combustion source. The FIu/(Flu+Pyr), BaA/(BaA+Chr) ratios analyzed the sources of PAHs in the sampling sites, including4oil combustion sources,6oil, firewood and coal mixed source,12high-temperature fuelwood combustion sources. The cluster analysis showed that the high ring PAHs monomer in Wenruitang River sediments mainly originated from heating sources, the low ring PAHs or alkyl substituted class PAHs mainly originated from natural sources and oil spill. Principal component analysis of PAHs sources showed that PAHs were related to the emission from diesel, natural gas and gasoline combustion. This principal component can be regarded as traffic related pollution source, fuelwood class combustion source and volatile petroleum-related products source. Ant/(Ant+Phe) characteristic ratios illustrated there were six sites for the petroleum-based pollution sources. FIu/(FIu+Pyr) ratio illustrated source of fuelwood class combustion accounted for75.8%, and also the presence of oil burning and oil spill source. FIu/(FIu+Pyr), BaA/(BaA+Chr) ratio showed that82.8%of the samples mainly originated from the burning of fuelwood substance, the combustion and leak of petroleum substances mixed sources accounted for17.2%. TheFIu/(Flu+Pyr), Inp/(Inp+BghiP)eigenvalue showed that55%of the sampling sites were fuelwood combustion sources, the remaining were oil spill source.
(8) The biological toxicity was measured by Qinghai Vibrio (Q7) against the surface water, interstitial water and sediment of Wenruitang River. Results showed that the average luminous intensity of the surface water was80.9%, belonging to slightly toxic; the average luminous intensity of interstitial water was69.7%, belonging to medium toxicity; the average luminous intensity of sediment was63.3%, belonging to medium toxicity. The order of relative luminous intensity was surface water>interstitial water>sediment. According to tropical Xenopus placed in sediment leaching, the toxicity results showed that the average hatching rate was75.98%, the average survival rate was83.77%, the average teratogenic rate was16.60%, and the average length was3.58cm. Sampling sites with complex pollution sources and serious pollution level had more significant toxic effect to the Xenopus embryo growth and development, whereas sampling sites with simple pollution source or sites in the river source area had less significant biological toxicity.
温瑞塘河是温州市最大的城市河网,被温州人民称为“母亲河”。温州市中小企业及家庭作坊式生产十分发达,在生产过程中由于管理松散而导致的污染物无序排放,进入水环境形成污染。本研究在国家重大水专项课(2009ZX07317-006);国家自然基金委青年科学基金(41101471)支助下,以温瑞塘河为研究对象,通过对上覆水、间隙水、沉积物中持久性有毒物质检测分析,利用发光细菌与热带爪蟾胚胎表征水环境生物毒性,利用数理统计分析方法解析持久性有毒物质的污染来源。揭示温瑞塘河水环境中持久性有毒物质(Cd、Cr、Pb、Hg、As、Cu、 Zn、Ni、PAHs)的空间分布特征、污染来源,水环境生物毒性及在模式生物的表现,水环境受污染程度与生态风险,为温瑞塘河水环境污染治理、水资源可持续利用与管理提供理论参考。本研究主要得到以下结论：
(1)在温瑞塘河上覆水与间隙水中重金属元素含量平均值大于地表水V标准,表明河流受到重金属污染,上覆水中Cd、Hg、Cr、Mn、Ni、Cu重金属元素含量低于间隙水,Zn元素例外,部分采样点上覆水中重金属含量高于间隙水,表明部分区域仍存在高浓度重金属污染。在温瑞塘河沉积物中各重金属元素的区间值(mg/kg)Hg(0.18～7.31)、Cd(0～149.53)、Cr(43.9～1892.70)、Pb(17.31～162.93)、As(2.12-17.79)、Cu(19.23-3393.81)、Zn(119.27-4934.87)、Ni(16.72～1646.09)。重金属Cd、Zn元素含量最高点位于温瑞塘河主干河道城市与工业集中区及支流河道的汇流区,其次为冶炼、电镀小企业集中的三垟湿地人口聚集区,支流源头区、农业及城市远郊区低。柱状样重金属垂直分布特征显示,重金属污染受农业污染源的影响在减轻,但农业面源污染仍存在,工业污染源、生活污染源污染呈增长趋势。Cd、Cr、Pb、Cu、Zn、Ni、Fe重金属元素形态为残渣态高于其他形态,可被生物利用有效态为Cd(66.75%)>Mn(65.90%)>Ni(63.55%)>Cu(60.24%)>Pb(59.67%)>Zn(58.61%)>Cr(54.70%)>Fe(23.69%)。
(2)沉积物单一重金属元素污染指数(Cfi)的评价结果为Cd(76.92)>Cu(17.4)>Hg(10.66)>Zn(9.19)>Ni(5.69)>Cr(4.30)>As(1.46)>Pb(1.43)。综合污染指数(Cd)评价受到重金属严重污染的采样点达14个,受重污染采样点为7个中污染采样点为8个,严重污染的采样点中Cd、Cu、Hg、Zn、Ni元素属严重污染状态。重金属的潜在生态危害指数(Eri)评价值为Cd(2307.47)>Hg(426.25)>Cu(87.03)>Ni(28.45)>As(14.58)>Zn(9.19)>Cr(8.60)>Pb(7.14)。重金属的生态风险指数RI结果显示采样点达极强生态风险点17个,强生态风险点7个,其中8##点生态风险最强,25#点生态风险最低点,河道沉积物受重金属Hg、Cd的污染存在很强的潜在生态风险可能。
(3)沉积物中重金属元素平均富集指数顺序为Cd(126.7)>Cu(33.1)>Zn(16.3)>Hg(14.71)>Ni(10.7)>Cr(7.80)>As(2.63)>Pb(2.6),其中As、Pb元素属于中污染,Cr、Ni、Hg、Zn属于偏重污染,Cu属于重污染,Cd属于严重污染。整个河道沉积物受Cd、Hg污染采样点区域最多,处于偏重污染程度的采样点百分比>75.86%,重金属元素As、Pb对沉积物污染最轻,其处于偏重污染程度的采样点百分比<6.90%。在内梅罗污染指数基础上建立的综合地累积指数评价表明沉积物受到Hg、Cd、Cu、Zn,Ni和Cr污染,采样点区域污染程度依次为机械工业园区>主河道城市区>三垟湿地区>城市周边区>水源地区。
(4)温瑞塘河的重金属污染主要来自于人为活动的影响,其重金属人为贡献率为Hg(86.62%)>Cd(81.20%)>Zn(80.59%)>Cu(75.86%)>Ni(68.12%)>Cr(64.26%)>As(54.7%)>Pb(45.78%),相关性分析与主成分分析表明Hg、Cd、Cu、Zn、Ni和Cr具有极显著相关性,来源以人为源为主,但也受到地球化学组成影响。
(5)多环芳烃在上覆水样中的含量Mean=128.13ng.L-1、Min=28.91ng.L-1、 Max=440.04ng.L-1,结构主要由低环(2+3)组成,PAHs含量机械工业园区域,城市生活与工厂混杂区域,城市生活旧城区域的含量较高。间隙水样的PAHs含量为Mean=631.87ng.L-1、Min=57.56ng.L-1、Max=1628.50ng.L-1,平均值大于上覆水样,结构以低环(2+3)为主。沉积物中PAHs含量Mean=1314.58ng.g-1、 Min=152.85ng.g-1、Max=3826.80ng.g-1,PAHs单体主要由2-6环组成,低环(2+3)结构平均占37.37%,中环(4)结构平均占37.41%,高环(5+6)结构平均占25.22%。PAHs在沉积物中的含量顺序为机械工业园区、城市生活与工厂混杂区、城市生活旧城区、支流河道交汇区、干流区与源头区。沉积物分层柱状样的PAHs含量在1#、3#、10#、14#、18#、20#点第一层高于第二和第三层,表明其污染日前处于加重趋势,2#、4#、7#、15#、16#、19#、21#、23#点第一层低于第二层或第三层,表明污染在降低。
(6)温瑞塘河上覆水水样的TEQ值范围在0.02-16.15ng.L-’,平均值2.62ng.L-1,平均值低于地表水质环境标准的2.8ng'L-1,毒性当量处于安全防范之内,在采样点中高于水质标准点7个,这些点具有较高生态风险。水环境中最小风险值范围15.42～1684.28,平均值为315.06,最大风险值范围0.15-16.84,平均值3.15,属高风险等级点4个,属中等风险等级点17个点,属低风险等级8个点沉积物中PAHs单体浓度值没有点超过生态效应值ERM,PAHs单体易发生生态风险的可能性小。沉积物毒性当量法的生物毒性区间(9.49-1331.09ng.g-1)平均值为158.2ng.g-1,沉积物最小风险商值平均值为438.99,风险商值区间为55.36～2833.31,属中等风险及以上样点达82.8%,具有发生潜在生态风险的可能。
(7)聚类分析与主成分分析表明温瑞塘河水样中PAHs单体的中高环由发热源产生,2-3环低分子量或者烷基取代类PAHs来自自然源或石油泄漏等。由FIu/(Flu+Pyr), Ant/(Ant+Phe)比值表明多环芳烃主要来源为燃烧来源,其中石油燃烧源占23.1%,其余为薪材等燃烧热源为76.9%,由FIu/(Flu+Pyr), BaA/(BaA+Chr)比值分析采样点PAHs来源,石油燃烧源4个,石油、薪材、煤混合源6个,高温薪材燃烧源12个。利用聚类分析表明温瑞塘河沉积物的PAHs来源中高环单体主要是发热源产生,2-3环低分子量或者烷基取代类PAHs主要来自自然源-石油泄露等,由主成分分析沉积物中PAHs污染来源,主成分分析与柴油车和天然气、汽油燃烧排放相关,该主成分可视为交通和与交通相关的污染来源,存在薪材类燃烧与石油相关产品挥发或泄漏源。由Ant/(Ant+Phe)特征比值显示有6个点为石油类污染源,FIu/(FIu+Pyr)比值显示薪材类燃烧源占75.8%,也存在石油燃烧与石油泄漏源。由FIu/(FIu+Pyr), BaA/(BaA+Chr)比值可知,主要由薪材类物质的燃烧的源点占82.8%,石油类物质的燃烧与泄漏混合源占17.2%。由FIu/(Flu+Pyr), Inp/(Inp+BghiP)特征值可知,55%的点为薪材燃烧源,其余为石油泄漏源。
(8)利用青海弧菌(Q7)对温瑞塘河上覆水,间隙水,沉积物生物毒性研究结果为上覆水样的平均发光强度为80.9%,属轻微毒性,间隙水相对发光强度的平均值69.7%,属中等生物毒性,沉积物相对发光强度的平均值63.3%,属中等生物毒性,上覆水相对发光强度>间隙水相对发光强度>沉积物的相对发光强度。沉积物浸出液对热带爪蟾胚胎发育毒性结果平均孵化率为75.98%,平均成活率为83.77%,平均致畸率为16.60%,平均体长为3.58cm。采样点污染源复杂与污染严重采样点对爪蟾胚胎发育生长毒性大,河流源头区及污染源单一采样点生物毒性小。
With the social and economic development, more and more pollutants with complex components are produced by human activity and natural process. Some trace pollutants which are persistent and biotoxic pose serious threat to the aquatic environmental. Persistent toxic substances are contaminants of strong biotoxicity and ecotoxicity, which are difficult to be degraded in the environment and constantly accumulate, enrich and magnify through the food chain in the ecosystem. Persistent toxic substances (PTS) can transport long distance in large scale via solid, gas and liquid. When PTS enter aquantic environment, they can affect living organisms directly through the overlying water, and also transport and transform among the overlying water-gap water-sediment through physical, chemical and biological processes of the water bodies. Thus, PTS have lasting impacts on the quality of the aquantic environment and furtherly affect the safety of the aquatic ecosystem. The persistent organic pollutants and heavy metal contaminant, two kinds of typical PTS in the aquatic environment, are hazardous to human beings and the nature since their impacts could be far-reaching and significant and their remediation is either hard and slow by nature process or costly and imperfect by artificial measures. Therefore, PTS in aquatic environment have been highly concerned worldwide.
Wenruitang River, the "mother river" called by the local people, is the largest urban river network in Wenzhou City. Wenzhou is famous for its small-medium sized enterprises and family workshops, pollutants are disorderly discharged to the aquatic environment in the production process due to the loose environmental management. With the support of the National Major Project (2009ZX07317-006) and the National Natural Science Youth Foundation of China (41101471), this dissertation took Wenruitang River as the research object, investigated the PTS in the surface water, pore water and sediments from Wenruitang River by chemical analysis, determined the PTS pollution sources through statistical analysis, assessed the biological toxicity of the PTS via light-emitting bacteria and tropical Xenopus embryos. It revealed the spatial distribution characteristics of PTS (Cd, Cr, Pb, Hg, As, Cu, Zn, Ni and PAHs) in Wenruitang River, pollution sources, PTS biological toxicity and the response of model organisms to PTS, assessed the contamination degree and ecological risk of PTS in Wenruitang River, hopefully to provide a theoretical reference for river pollution treatment and the sustainable use and management of river water resources. The major conclusions of this research are listed as follows:
(1) The average heavy metal content in the surface water and pore water from Wenruitang River was higher than the corresponding value in the level V of the surface water standard of China, which showed that the river was polluted by heavy metals. The content of Cd, Hg, Cr, Mn, Ni and Cu in the surface water was less than that in the pore water. Zn was an exception, for its concentration in the surface water from some of the sampling sites was higher than that in the pore water from the same place. The interval values (mg/kg) of heavy metals from the sediments of Wenruitang River were:Hg (0.18～7.31), Cd (0～149.53), Cr (43.9～1892.70), Pb (17.31～162.93), As (2.12～17.79), Cu (19.23～3393.81), Zn (119.27～4934.87) and Ni (16.72～1646.09). The sampling site with the maximum Cd and Zn contents located in the main channel of Wenruitang River where residential area and industrial area were overlapped, following by Sanyang wetland area where small smelting and plating factories used to concentrated there, and the minimum Cd and Zn contents in agriculture and exurban area. Vertical distribution characteristics of heavy metal in core sediment samples showed that heavy metal pollution caused by agricultural sources was reduced while pollution caused by industrial sources and residential sources were increasing. Heavy metals Cd, Cr, Pb, Cu, Zn, Ni and Fe were mostly in the form of residual fraction rather than other forms. The bioavailable state of these heavy metals were Cd (66.75%)> Mn (65.90%)> Ni (63.55%)> Cu (60.24%)> Pb (59.67%)> Zn (58.61%)> Cr (54.70%)> Fe (23.69%).
(2) The evaluation result of the sediment single element pollution index (Cf1) was Cd (76.92)> Cu (17.4)> Hg (10.66)> Zn (9.19)> Ni (5.69)> Cr (4.30)> As (1.46)> Pb (1.43). The evaluation results of integrated Pollution Index (Cd) indicated that the numer of seriously, heavily and moderately polluted sampling sites was14,7and8, respectively. Among the seriously polluted sampling sites, Cd, Cu, Hg, Zn, and Ni belonged to the serious pollution level. The order of potential ecological risk index (Er1) was Cd (2307.47)> Hg (426.25)> Cu (87.03)> Ni (28.45)> As (14.58)> Zn (9.19)> Cr (8.60)> Pb (7.14). The results of the ecological risk index RI showed that there were17sampling sites of extremely strong ecological risk,7sampling sites of strong ecological risk and no site of low ecological risk. The highest ecological risk appeared at sampling site8#while the lowest was at sampling site25#. Hg and Cd had strong potential ecological risk.
(3) The order of the average enrichment index of heavy metals in the sediment was Cd (126.7)> Cu (33.1)> Zn (16.3)> Hg (14.71)> Ni (10.7)> Cr (7.80)> As (2.63)> Pb (2.6). According to this order, As and Pb belonged to moderate pollution, Cr, Ni, Hg and Zn belonged to moderate to heavy pollution, Cu belonged to heavy pollution, Cd belonged to serious pollution. The entire river sediments were mostly polluted by Cd and Hg in term of polluted area with more than75.86%sampling sites were no less than the level of moderately to heavily contaminated, whereas As and Pb were leastly polluted with less than6.90%sampling sites were in the level of more serious pollution. Based on the Nemerow Pollution Index, a comprehensive geoaccumulation index was established. The geoaccumulation index showed that the sediments were polluted by Hg, Cd, Cu, Zn, Ni and Cr. The pollution level order of different region was machinery industrial park> main river city downton section> Sanyang Wetland> suburban areas> drinking water source areas.
(4) Heavy metal pollution in Wenruitang River mainly affected by human activities. The anthropogenic contribution rate of each heavy metal was Hg (86.62%)> Cd (81.20%)> Zn (80.59%)> Cu (75.86%)> Ni (68.12%)> Cr (64.26%)> As (54.7%)> Pb (45.78%). The correlation analysis and principal component analysis indicated that Hg, Cd, Cu, Zn, Ni and Cr were significantly correlated. Heavy metals in Wenruitang River were mainly originated from anthropogenic sources, and affected by geochemical process at the mean time.
(5) The minimum, maximum and mean concentration of polycyclic aromatic hydrocarbons in the surface river water was28.91ng.L-1,440.04ng.L-1and128.13ng.L-1, respectively. PAHs structure composed mainly by low ring (2+3). PAHs had higher concentration in machinery industrial park area, residential and industrial mixed area as well as the old city area. The maximum, mean and minimum concentrations of PAHs in interstitial water were1628.50ng.L-1,631.87ng.L-1and57.56ng.L-1, respectively. The average PAHs concentration in the interstitial water was greater than that in the surface water samples. The PAHs structure composed mainly by the low ring (2+3). The minimum, maximum and mean contents of PAHs in the sediments were152.85ng.g-1,3826.80ng.g-1and1314.58ng.g-1, respectively. PAHs monomer mainly composed by2～6rings, low ring (2+3) structure accounted for37.37%by average, middle ring (4) structure accounted for37.41%, high ring (5+6) structure accounted for25.22%. The order of PAHs content in sediments were machinery industrial park area> residential and industrial mixed area> the old city area> tributary confluence area> the main river stream and the river source area.
The PAHs content in the sediment column sample showed that the first layer had higher PAHs than the second and third layers from samples1#,3#,10#,14#,18#and20#, which revealed that the pollution was aggravating. PAHs content in the first layer was lower than that in the second and third layers from samples2#,4#,7#,15#,16#,19#,21#and23#, which indicated that the pollution was reducing.
(6) The TEQ values of surface water samples of Wenruitang River ranged from0.02to16.15ng.L-1. The average value was2.62ng.L-1, which is lower than2.8ng.L-1defined by the surface water quality environmental standards, meaning that the toxic equivalence was in security. There were7sampling sites with TEQ value higher than the surface water quality standards. These sampling sites would face higher ecological risk. The minimum risk value ranged from15.42to1684.28with the average value of315.06. The maximum risk value ranged from0.15to16.84with the average of3.15. There were4high-risk rating sties,17medium risk rating sites and8low risk rating sites. PAHs monomer concentration in sediments exceeding the ecological effects ERM was not found, so PAHs monomer in sediments was not liketly to induce ecological risk. The average biological toxicity by sediment toxicity equivalent methodwas158.2ng.g-1(ranged from9.49to1331.09ng.g-1). The average sediment minimum risk quotient is438.99, the risk quotient value ranged from55.36to2833.31. The samples had at least medium risk accounted for82.8%, indicating the possibility of potential ecological risk.
(7) The cluster analysis and principal component analysis demonstrated that middle and high ring of PAHs monomer was generated by the heat source, the low ring with low molecular weight or alkyl substituted class of PAHs was originated from natural sources or oil spill. The FIu/(Flu+Pyr), Ant/(Ant+Phe) ratios indicated that the main source of polycyclic aromatic hydrocarbons was combustion sources, including23.1%oil combustion sources and76.9%fuelwood combustion source. The FIu/(Flu+Pyr), BaA/(BaA+Chr) ratios analyzed the sources of PAHs in the sampling sites, including4oil combustion sources,6oil, firewood and coal mixed source,12high-temperature fuelwood combustion sources. The cluster analysis showed that the high ring PAHs monomer in Wenruitang River sediments mainly originated from heating sources, the low ring PAHs or alkyl substituted class PAHs mainly originated from natural sources and oil spill. Principal component analysis of PAHs sources showed that PAHs were related to the emission from diesel, natural gas and gasoline combustion. This principal component can be regarded as traffic related pollution source, fuelwood class combustion source and volatile petroleum-related products source. Ant/(Ant+Phe) characteristic ratios illustrated there were six sites for the petroleum-based pollution sources. FIu/(FIu+Pyr) ratio illustrated source of fuelwood class combustion accounted for75.8%, and also the presence of oil burning and oil spill source. FIu/(FIu+Pyr), BaA/(BaA+Chr) ratio showed that82.8%of the samples mainly originated from the burning of fuelwood substance, the combustion and leak of petroleum substances mixed sources accounted for17.2%. TheFIu/(Flu+Pyr), Inp/(Inp+BghiP)eigenvalue showed that55%of the sampling sites were fuelwood combustion sources, the remaining were oil spill source.
(8) The biological toxicity was measured by Qinghai Vibrio (Q7) against the surface water, interstitial water and sediment of Wenruitang River. Results showed that the average luminous intensity of the surface water was80.9%, belonging to slightly toxic; the average luminous intensity of interstitial water was69.7%, belonging to medium toxicity; the average luminous intensity of sediment was63.3%, belonging to medium toxicity. The order of relative luminous intensity was surface water>interstitial water>sediment. According to tropical Xenopus placed in sediment leaching, the toxicity results showed that the average hatching rate was75.98%, the average survival rate was83.77%, the average teratogenic rate was16.60%, and the average length was3.58cm. Sampling sites with complex pollution sources and serious pollution level had more significant toxic effect to the Xenopus embryo growth and development, whereas sampling sites with simple pollution source or sites in the river source area had less significant biological toxicity.
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