长江口南岸滨岸带底泥中重金属的生物有效性及其再悬浮
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摘要
本论文选取长江口南岸吴淞-浏河滨岸段作为典型区域,以有毒重金属Pb、Cd、Cr为主要研究对象,借助SEM与AVS的差值和比值方法对长江口吴淞-浏河带沉积物中的重金属进行生物有效性评价,进而来判断沉积物中的有效态重金属对底栖生物的危害程度;进行潮周期的定点现场观测,研究潮周期过程中物理再悬浮及动力、pH、盐度等环境条件耦合影响下底泥中重金属(Pb、Cr、Cd)的潮周期变化特征;同时利用自制的再悬浮装置(PES)进行室内模拟再悬浮试验,研究重金属(Pb、Cr、Cd)在沉积物-上覆水之间的迁移转化过程。主要得到以下几条结论:
1)长江口吴淞-浏河滨岸带Pb、Cr、Cd、Hg、As的平均含量分别为33.1μg·g~(-1)、56.6μg·g~(-1)、0.4μg·g~(-1)、0.38μg·g~(-1)、40.0μg·g~(-1),其含量均超过上海市潮滩背景值;除Cr外,其它重金属含量均超过上海市土壤背景值。浏河口上游到江苏白茆附近沉积物和水体中Cd平均含量分别为0.189μg·g~(-1)、0.234μg·L~(-1),分别超过上海市潮滩背景值和2008年6月所采陈行水库水体Cd含量。长江口南岸存在重金属的岸边污染带。
2)由于上海腹地工业废水、生活污水的大量排放,使得长江口吴淞-浏河滨岸带沉积物中具有较高的SEM(Simultaneously Extracted Metals)和AVS(AcidVolatile Sulfides)含量,分别为0.20-1.37μmol·g~(-1)、0.20-0.80μmol·g~(-1),不同重金属的总量、SEM含量都超过了上海市土壤、潮滩重金属背景值,且该研究区域沉积物中以HCl淋滤相存在的重金属占主要形式;浏河口上游长江口南岸沿岸带主要以Cd污染为主,Cr、Pb含量均低于上海市土壤背景值,污染程度较小。
3)吴淞-浏河滨岸带沉积物中有机碳、含水率以及沉积物粒径本身是本研究区域中SEM与AVS含量的控制性环境因子;SEM/AVS比值及(SEM-AVS)差值的生物有效性评价结果表明,长江口吴淞-浏河滨岸带沉积物中重金属对水生生物均处于中等毒性水平,底泥的再悬浮作用会加强硫化物结合态重金属的释放,从而引起环境毒性。
4)潮周期现场观测过程中,水体流速的变化是控制底泥中重金属向水体释放的主要环境因子。另外,水体中各形态重金属的浓度变化还受其它外在环境因子的影响,如水温、pH、NO_3~-、DOC、DIC、NH_4~+、TN等是控制水体底层溶解态Cd的重要环境指标,DO、Eh是控制表层溶解态Cd和Pb环境因子;Cl~-是控制底层水体溶解态Pb的重要环境因子;Eh是控制表层水体溶解态Cr的重要环境因子,DO、NO_3~-是控制表层水体颗粒态Cr的重要环境因子,DOC是控制底层水体可溶性Cr的环境因子,电导率是控制底层颗粒态Cr的重要环境因子。
5)相关性分析发现,潮周期现场观测过程中溶解态Cd、Pb、Cr两两之间分别存在显著正相关关系;颗粒态Cd、Pb、Cr两两之间也存在显著正相关,且颗粒态重金属(Pb、Cr、Cd)与全量的Pb、Cr、Cd之间也存在显著相关性。这说明颗粒态的Pb、Cr、Cd具有相似的理化性质及物质来源。流速分别与颗粒态及总量重金属(Pb、Cr、Cd)均呈显著正相关关系。潮水动力对于水体颗粒态重金属的贡献具有不可忽视的作用。
6)通过对潮周期现场观测前后底泥柱状沉积物中重金属及其理化参数的含量对比发现,潮周期过程中底泥对Pb、Cr有富集效应;Cd、Fe、Mn的变化可能受孔隙水的影响较大;底泥中Cu、Ni向水体发生了释放;初步判断潮周期过程中动力扰动所影响到的底泥深度大约为0-5cm。
7)在受水体生物膜保护的作用下,水体中溶解态和颗粒态重金属含量呈波浪状的变化受重金属吸附的“泥沙效应”影响非常显著;在外界环境因子变化相对稳定的情况下,溶解态和颗粒态重金属在两相之间也会在短时间内达到浓度平衡;同现场潮周期观测结果相似,另外在个别时间点水体中两相态的重金属含量也受DOC、DO等环境因子的控制。
8)与潮周期现场观测结果有所不同的是,通过对比室内模拟再悬浮试验前后柱状沉积物中各重金属(Pb、Cr、Cd)及主要理化参数(硫化物、含水率、有机质)的变化,大部分试验结果证实沉积物确实向水体释放了重金属,但途径略有不同:或来源于沉积物经孔隙水向上覆水体的释放(pH模拟);或来源于水体生物膜上铁锰氧化物结合态重金属的释放(盐度模拟);或来源于两者的综合作用(pH、盐度耦合模拟,动力、盐度耦合模拟)。
9)与潮周期现场观测结果相似,室内模拟长江口底泥重金属再悬浮试验发现,在有水体生物膜存在的条件下,重金属吸附的“泥沙效应”对水体中重金属的迁移转化影响显著。硫化物的前后含量变化可以作为判断动力扰动到底泥深度的一个有力证据。
The intertidal flat in Wusong-Liuhe coastal zone in the Yangtze Estuary is a complex ecosystem influenced both by natural fators and strong human activities.In order to evaluate biological availability of heavy metals in sediments,acid volatile sulfides(AVS) and simultaneously extracted metals(SEM) of 37 surface sediments colleted from Wusong-Liuhe coastal zone in the Yangtze Estuary were determined. This is favourable for evaluating the toxicity level to human;a tidal cycle was observed nearby Chenghang reservoir to study resuspended release process of heavy metals(Pb,Cr and Cd) in sediments under the condition of different tidal dynamics and physical and chemical factors(such as pH and salinity).In addition,combined with results of spot observation,the effects of sediment resuspension for Pb,Cr and Cd at the sediment-water interface exchange at the sediment through different techniques of experimental simulation were discussed.
The main results gotten in the article are as follows:
1)The average content of Pb,Cr,Cd,Hg and As was 33.1μg·g~(-1),56.6μg·g~(-1), 0.4μg·g~(-1),0.38μg·g~(-1) and 40.0μg·g~(-1) of sediments in Wusong-Liuhe coastal zone. All heavy metals are above background values of heavy metals of mad flat in Shanghai.The content of all heavy metals exceed background value of heavy metals of soils in Shanghai except Cr.The average of Cd were 0.189μg·g~(-1), 0.234μg·L~(-1) in sediments and water from upwards Liu river estuary.The content of Cd in sedimens and water exceed the background value of heavy metals and the water of Chenhang reservoir in June,2008,respectively.There probably exists a polluted strip in Yangtze River south estuary.
2)The SEM contents of the surface sediments ranged from 0.20μmol·g~(-1) to 1.37μmol·g~(-1)(dry weight),with an average value of 0.74μmol·g~(-1);The AVS contents varied between 0.20-0.80μmol·g~(-1)(dry weight),with an average being 0.23μmol·g~(-1) of sediment in Wusong-Liuhe coastal zone.Both total contents of different heavy metal(Pb,Cr,Cd,Hg and As) and SEM are over background value of intertidal flat and soil in Shanghai.This is mainly contributed by waste from industry and daily life.The heavy metals combined with HCl is dominating form existed in study area.In upriver of Liuhe estuary,Cd is major contaminant, Pb and Cr are minor contaminant.
3)TOC,water level and medium particle size of the sediment are the main controlling environmental factors in study area.The ratio of SEM to AVS and the difference between SEM and AVS are used to assess the biological availability of sediment SEM content.The result shows that the SEM of the surface sediments at Wusong-Liuhe riparian zone in Yangtze Estuary had moderate toxicity to the aquatic life.Resuspended process of sediment will enhance the release of heavy metals which combined with sulfide and then arouse environmental toxicity.
4)During spot observation of tidal cycle,water velocity is the mainly controlled environmental factor for the release of heavy metal(Pb,Cr,Cd) in substrate sludge.In addition,water temperature,NO_3~-,DOC,DIC,NH_4~+,TN are predominate environmental factors which control dissolved Cd in bottom water, DO,Eh are important environmental factors which control dissolved Cd and Pb surface water.Cl~-is an important environmental factor which control dissolved Pb in bottom water.Eh is an important environmental factor which control dissolved Cr in surface water.DO and NO_3~-are predominate environmental factor which control particled Cr in surface water.DOC is an important environmental factor which control dissolved Cr in bottom water.EC is an important environmental factor which control particled Cr in bottom water.
5)Correlation analysis is an important way to weigh the relation between dissolved and particled heavy metals(Pb,Cr and Cd) during ticle cyc.Dissolved Cd has significant positive correlations with dissolved Pb and Cr.Particled Cd and total Cd also have this relation with particle Pb and Cr.It is a forceful evidence that particled Pb,Cr and Cd have similar physical and chemical properties and sources.Water velocity has significant positive correlations with particled Pb and Cr and total Pb,Cr and Cd.Tidal impetus has important effect to particled heavy metals of water.
6)In comparision with heavy metals(Pb,Cr,Cd,Cu,Ni,Mn,Fe and Mn) content and physics and chemical parameters of columnar sediments before and after tidal cyc,the bottom mud has concentration effect to Pb and Cr,the change of Cd,Fe and Mn are possibly effected by pore water,the bottom mud has a release of Cu and Ni to water.From the initial assessment,the bottom mud depth caused by perturbation affects probably is(0-5cm) initially during the moist cyclical process.
7)Under the protection of water biomembrane,the change of dissolved and particled heavy metals' concentration in water is mainly caused by“the silt effect”of heavy metals.When the change of external environmetal factors is relative stable,dissolved and particled heavy metals will be in short-lived balance condition.Moreover,DOC and DO will also controll the change of heavy metals in individual time.
8)In the process of indoor resuspension simulation,in contrast with heavy metals (Pb,Cr and Cd) content and physiochemical parameters(sulfide,moisture content, organic matter) of columnar sediments before and after resuspension experiment, most experiments mostly proved that sediment release heavy metals to water,but the way of resuspending has slight difference:or originates from the deposit after the pore water upward rehydrate body's release;or originates from the deposit pore water;or originates in the water body biomembrane the ferro manganese oxide compound union condition heavy metal release.
9)Lab-scale resuspending simulation of heavy metal in Changjiang delta bottom mud discovered that the heavy metals'“the silt effect”has remarkable effect to the heavy metals' migration and transformation activity in water body,under the water body biomembrane existence condition.The change of sulfide content can be a powerful evidence to judge the bottom mud depth disturbed by water momentum.
1)长江口吴淞-浏河滨岸带Pb、Cr、Cd、Hg、As的平均含量分别为33.1μg·g~(-1)、56.6μg·g~(-1)、0.4μg·g~(-1)、0.38μg·g~(-1)、40.0μg·g~(-1),其含量均超过上海市潮滩背景值;除Cr外,其它重金属含量均超过上海市土壤背景值。浏河口上游到江苏白茆附近沉积物和水体中Cd平均含量分别为0.189μg·g~(-1)、0.234μg·L~(-1),分别超过上海市潮滩背景值和2008年6月所采陈行水库水体Cd含量。长江口南岸存在重金属的岸边污染带。
2)由于上海腹地工业废水、生活污水的大量排放,使得长江口吴淞-浏河滨岸带沉积物中具有较高的SEM(Simultaneously Extracted Metals)和AVS(AcidVolatile Sulfides)含量,分别为0.20-1.37μmol·g~(-1)、0.20-0.80μmol·g~(-1),不同重金属的总量、SEM含量都超过了上海市土壤、潮滩重金属背景值,且该研究区域沉积物中以HCl淋滤相存在的重金属占主要形式;浏河口上游长江口南岸沿岸带主要以Cd污染为主,Cr、Pb含量均低于上海市土壤背景值,污染程度较小。
3)吴淞-浏河滨岸带沉积物中有机碳、含水率以及沉积物粒径本身是本研究区域中SEM与AVS含量的控制性环境因子;SEM/AVS比值及(SEM-AVS)差值的生物有效性评价结果表明,长江口吴淞-浏河滨岸带沉积物中重金属对水生生物均处于中等毒性水平,底泥的再悬浮作用会加强硫化物结合态重金属的释放,从而引起环境毒性。
4)潮周期现场观测过程中,水体流速的变化是控制底泥中重金属向水体释放的主要环境因子。另外,水体中各形态重金属的浓度变化还受其它外在环境因子的影响,如水温、pH、NO_3~-、DOC、DIC、NH_4~+、TN等是控制水体底层溶解态Cd的重要环境指标,DO、Eh是控制表层溶解态Cd和Pb环境因子;Cl~-是控制底层水体溶解态Pb的重要环境因子;Eh是控制表层水体溶解态Cr的重要环境因子,DO、NO_3~-是控制表层水体颗粒态Cr的重要环境因子,DOC是控制底层水体可溶性Cr的环境因子,电导率是控制底层颗粒态Cr的重要环境因子。
5)相关性分析发现,潮周期现场观测过程中溶解态Cd、Pb、Cr两两之间分别存在显著正相关关系;颗粒态Cd、Pb、Cr两两之间也存在显著正相关,且颗粒态重金属(Pb、Cr、Cd)与全量的Pb、Cr、Cd之间也存在显著相关性。这说明颗粒态的Pb、Cr、Cd具有相似的理化性质及物质来源。流速分别与颗粒态及总量重金属(Pb、Cr、Cd)均呈显著正相关关系。潮水动力对于水体颗粒态重金属的贡献具有不可忽视的作用。
6)通过对潮周期现场观测前后底泥柱状沉积物中重金属及其理化参数的含量对比发现,潮周期过程中底泥对Pb、Cr有富集效应;Cd、Fe、Mn的变化可能受孔隙水的影响较大;底泥中Cu、Ni向水体发生了释放;初步判断潮周期过程中动力扰动所影响到的底泥深度大约为0-5cm。
7)在受水体生物膜保护的作用下,水体中溶解态和颗粒态重金属含量呈波浪状的变化受重金属吸附的“泥沙效应”影响非常显著;在外界环境因子变化相对稳定的情况下,溶解态和颗粒态重金属在两相之间也会在短时间内达到浓度平衡;同现场潮周期观测结果相似,另外在个别时间点水体中两相态的重金属含量也受DOC、DO等环境因子的控制。
8)与潮周期现场观测结果有所不同的是,通过对比室内模拟再悬浮试验前后柱状沉积物中各重金属(Pb、Cr、Cd)及主要理化参数(硫化物、含水率、有机质)的变化,大部分试验结果证实沉积物确实向水体释放了重金属,但途径略有不同:或来源于沉积物经孔隙水向上覆水体的释放(pH模拟);或来源于水体生物膜上铁锰氧化物结合态重金属的释放(盐度模拟);或来源于两者的综合作用(pH、盐度耦合模拟,动力、盐度耦合模拟)。
9)与潮周期现场观测结果相似,室内模拟长江口底泥重金属再悬浮试验发现,在有水体生物膜存在的条件下,重金属吸附的“泥沙效应”对水体中重金属的迁移转化影响显著。硫化物的前后含量变化可以作为判断动力扰动到底泥深度的一个有力证据。
The intertidal flat in Wusong-Liuhe coastal zone in the Yangtze Estuary is a complex ecosystem influenced both by natural fators and strong human activities.In order to evaluate biological availability of heavy metals in sediments,acid volatile sulfides(AVS) and simultaneously extracted metals(SEM) of 37 surface sediments colleted from Wusong-Liuhe coastal zone in the Yangtze Estuary were determined. This is favourable for evaluating the toxicity level to human;a tidal cycle was observed nearby Chenghang reservoir to study resuspended release process of heavy metals(Pb,Cr and Cd) in sediments under the condition of different tidal dynamics and physical and chemical factors(such as pH and salinity).In addition,combined with results of spot observation,the effects of sediment resuspension for Pb,Cr and Cd at the sediment-water interface exchange at the sediment through different techniques of experimental simulation were discussed.
The main results gotten in the article are as follows:
1)The average content of Pb,Cr,Cd,Hg and As was 33.1μg·g~(-1),56.6μg·g~(-1), 0.4μg·g~(-1),0.38μg·g~(-1) and 40.0μg·g~(-1) of sediments in Wusong-Liuhe coastal zone. All heavy metals are above background values of heavy metals of mad flat in Shanghai.The content of all heavy metals exceed background value of heavy metals of soils in Shanghai except Cr.The average of Cd were 0.189μg·g~(-1), 0.234μg·L~(-1) in sediments and water from upwards Liu river estuary.The content of Cd in sedimens and water exceed the background value of heavy metals and the water of Chenhang reservoir in June,2008,respectively.There probably exists a polluted strip in Yangtze River south estuary.
2)The SEM contents of the surface sediments ranged from 0.20μmol·g~(-1) to 1.37μmol·g~(-1)(dry weight),with an average value of 0.74μmol·g~(-1);The AVS contents varied between 0.20-0.80μmol·g~(-1)(dry weight),with an average being 0.23μmol·g~(-1) of sediment in Wusong-Liuhe coastal zone.Both total contents of different heavy metal(Pb,Cr,Cd,Hg and As) and SEM are over background value of intertidal flat and soil in Shanghai.This is mainly contributed by waste from industry and daily life.The heavy metals combined with HCl is dominating form existed in study area.In upriver of Liuhe estuary,Cd is major contaminant, Pb and Cr are minor contaminant.
3)TOC,water level and medium particle size of the sediment are the main controlling environmental factors in study area.The ratio of SEM to AVS and the difference between SEM and AVS are used to assess the biological availability of sediment SEM content.The result shows that the SEM of the surface sediments at Wusong-Liuhe riparian zone in Yangtze Estuary had moderate toxicity to the aquatic life.Resuspended process of sediment will enhance the release of heavy metals which combined with sulfide and then arouse environmental toxicity.
4)During spot observation of tidal cycle,water velocity is the mainly controlled environmental factor for the release of heavy metal(Pb,Cr,Cd) in substrate sludge.In addition,water temperature,NO_3~-,DOC,DIC,NH_4~+,TN are predominate environmental factors which control dissolved Cd in bottom water, DO,Eh are important environmental factors which control dissolved Cd and Pb surface water.Cl~-is an important environmental factor which control dissolved Pb in bottom water.Eh is an important environmental factor which control dissolved Cr in surface water.DO and NO_3~-are predominate environmental factor which control particled Cr in surface water.DOC is an important environmental factor which control dissolved Cr in bottom water.EC is an important environmental factor which control particled Cr in bottom water.
5)Correlation analysis is an important way to weigh the relation between dissolved and particled heavy metals(Pb,Cr and Cd) during ticle cyc.Dissolved Cd has significant positive correlations with dissolved Pb and Cr.Particled Cd and total Cd also have this relation with particle Pb and Cr.It is a forceful evidence that particled Pb,Cr and Cd have similar physical and chemical properties and sources.Water velocity has significant positive correlations with particled Pb and Cr and total Pb,Cr and Cd.Tidal impetus has important effect to particled heavy metals of water.
6)In comparision with heavy metals(Pb,Cr,Cd,Cu,Ni,Mn,Fe and Mn) content and physics and chemical parameters of columnar sediments before and after tidal cyc,the bottom mud has concentration effect to Pb and Cr,the change of Cd,Fe and Mn are possibly effected by pore water,the bottom mud has a release of Cu and Ni to water.From the initial assessment,the bottom mud depth caused by perturbation affects probably is(0-5cm) initially during the moist cyclical process.
7)Under the protection of water biomembrane,the change of dissolved and particled heavy metals' concentration in water is mainly caused by“the silt effect”of heavy metals.When the change of external environmetal factors is relative stable,dissolved and particled heavy metals will be in short-lived balance condition.Moreover,DOC and DO will also controll the change of heavy metals in individual time.
8)In the process of indoor resuspension simulation,in contrast with heavy metals (Pb,Cr and Cd) content and physiochemical parameters(sulfide,moisture content, organic matter) of columnar sediments before and after resuspension experiment, most experiments mostly proved that sediment release heavy metals to water,but the way of resuspending has slight difference:or originates from the deposit after the pore water upward rehydrate body's release;or originates from the deposit pore water;or originates in the water body biomembrane the ferro manganese oxide compound union condition heavy metal release.
9)Lab-scale resuspending simulation of heavy metal in Changjiang delta bottom mud discovered that the heavy metals'“the silt effect”has remarkable effect to the heavy metals' migration and transformation activity in water body,under the water body biomembrane existence condition.The change of sulfide content can be a powerful evidence to judge the bottom mud depth disturbed by water momentum.
引文
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