岱海与达里诺尔湖重金属的环境地球化学研究
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摘要
天然水是一个包括多种无机物和有机物的复杂的多相电解质系统。重金属作为这个系统的组分,其化学行为必然要受到整个系统的影响。湖泊沉积物中重金属污染是世界各国面临的环境问题之一。重金属是自然界中广泛存在的物质之一,可作为水体污染的指示剂,具有反应水—沉积物系统状况的意义,直接和间接地威胁着“自然—经济—社会”这一复合生态系统。因此,对湖泊沉积物中重金属进行环境风险评价是判识重金属对生态环境的影响具有重要的现实意义。
本文以中国北方的岱海和达里诺尔为研究对象,以2个湖泊沉积物中重金属的形态分析为基础,系统开展了不同地质背景、不同水质类型湖泊沉积物中重金属赋存形态、AVS与SEM含量及分布特征的对比研究,探讨了重金属在这两个湖泊沉积物中的迁移转化规律,揭示了岱海和达里诺尔湖泊沉积物中重金属形态分布特征与生物有效性的关系,利用基于重金属总量、形态学和ΣSEM/AVS比值法等评价方法,预测和判识了岱海和达里诺尔沉积物中重金属污染可能存在的潜在危害性,得出如下主要结论：
1.研究表明,岱海和达里诺尔湖水质类型分别为氯化物类钠组Ⅰ型水和碳酸盐类钠组Ⅰ型水。2个湖泊矿化度均从上世纪90年代末始逐渐增加,至2011年2个湖泊的氯离子和钠离子均有大幅增长,尤以岱海钙镁比例的失调须引起关注。
2.形态分析表明,铁锰氧化物结合态是岱海沉积物Pb(占总量的43.56%)、Cd(占总量的65.25%)的主导形态,碳酸盐结合态是达里诺尔沉积物Pb(占总量的36.62%)、Cd(占总量的43.89%)的主导形态。总体上,达里诺尔沉积物中Cu、Pb、Zn、Cd的生物有效态含量高于岱海,揭示达里诺尔沉积物中4种重金属的潜在生态风险较高。2个湖泊沉积物中生物有效态重金属的主导形态体现了4种重金属元素的地球化学特性的差异性及2个湖泊水质类型和演化阶段的差异性。
3.研究表明,2个湖泊沉积物中SEM/AVS比值的平均值都大于1,都可能对底栖生物产生毒性作用。尽管岱海硫酸根的含量(170.30mg/L)远小于达里诺尔的硫酸根含量(328.28mg/L),但达里诺尔高盐度(6759.20mg/L)、高碱度(3201.20mg/L)和高pH(9.5)抑制了硫酸盐还原细菌的活性使硫酸根得以保存下来,导致达里诺尔的AVS含量远小于岱海AVS,揭示了达里诺尔沉积物中AVS对重金属的控制作用较弱。此外,岱海南岸建有火力发电厂,其排放的冷却水中含有大量硫酸根离子且岱海水中氧化还原电位较低(平均Eh为-139.27mV),导致大量AVS产生。
4.形态分析、SEM/AVS值及多种综合评价的结果均显示,2个湖泊沉积物中Cd和Pb的潜在生态风险最大,是水环境重金属污染中优先控制的污染物。
5.两个湖泊沉积物中重金属污染用三类评价方法评价的结果并不完全一致,基于重金属总量的评价方法(除沉积物质量基准方法)的评价结果基本一致,且岱海沉积物污染水平高于达里诺尔；基于形态的评价方法中达里诺尔沉积物污染水平高于岱海；而用SEM/AVS的评价结果相近(岱海和达里诺尔沉积物中SEM/AVS分别为1.46、1.55)。这可能与这些评价方法的自身特色、适用范围及其局限性有关,例如基于重金属总量的评价方法的缺点是基准值设定的科学性和合理性有时难以保证。因此,有必要采用多种方法进行综合评价,以便相互补充。
Natural water is a complex multiphase electrolyte system that contains a variety of inorganic and organic matter. AS heavy metals are components of this system, its chemical behavior is necessarily affected by the whole system. Heavy metals pollution in lake sediment is one of the environmental problems facing the world. As one of the widely existing in the nature, heavy metals can be the indicator of water pollution, reflect condition of water-sediment system, while threaten the complex ecosystem of "nature-economy-society" directly or indirectly. So it has important practical significance to recognize the impact of heavy metals on the ecological environment using environmental risk assessment of heavy metals in lake sediment.
The objects of this study are sediments of Daihai Lake and Dalinuoer Lake in northern China. Based on the speciation analysis of heavy metals in both lake sediments, the speciation of heavy metals and the contents and distribution characteristics of AVS and SEM in lake sediment which have different geological background and different types of water quality are compared systematically; the transition and transform rule of heavy metals are discussed in both lake sediments; the relationship between distribution characteristics of speciation and the biological effectiveness of heavy metals in both lake sediments are revealed; being used assessment methods such as the method that is based on the total amount and speciation of heavy metals and∑SEM/AVS ratio, potential hazards of heavy metal pollution in both lake sediments are predicted and sentenced. The major conclusions are as following:
1. The water quality type of Daihai Lake and Dalinuoer Lake is different. The former is I type water of sodium chloride class group, and the latter is I type water of sodium carbonate group. The dissolve solids of both lake have gradually increased since the beginning of the late1990s. Up until2011, the Cl" and Na+of both lake have increased significantly, and the imbalance of Ca/Mg ratio of Daihai Lake especially should be paid close attention.
2. Speciation analysis shows that the dominant speciation of Pb (43.56%of the total) and Cd (65.25%of the total) in the sediments of Daihai Lake is iron and manganese oxides, while the dominant speciation of Pb (36.62%of the total) and Cd (43.89%of the total) in the sediments of Dalinuoer Lake is carbonates. Overall, the bio-available speciation of heavy metals (including Cu,Pb,Zn,Cd) in Dalinuoer Lake sediments is higher than those in Daihai Lake, which reveal that potential ecological risk of those four kinds of heavy metals in Dalinuoer Lake sediments is higher. The dominant speciations of those four kinds of heavy metals in the lakes not only show the difference of the geochemical features among four kinds of heavy metals, but also reveal the difference of lake water quality types and evolution stages between two lakes.
3. Study shows that the average SEM/AVS ratio in both lake sediments are greater than1. So they would have toxic effects on benthos. Although the SO42-concentration (170.30mg/L) of Daihai Lake is far less than Dalinuoer Lake (328.28mg/L), the high salinity (6759.20mg/L), high basicity (3201.20mg/L) and high pH (9.5) of Dalinuoer Lake inhibit the activity of sulfate reducing bacteria so as to make SO4-2be preserved, which leads to the AVS concentration of Dalinuoer Lake is far less than Daihai Lake. This result reveals that the AVS content of Dalinuoer Lake sediments have weak control effects to the heavy metals. In addition, a lot of SO42-in the cooling water discharged by a coal-fired power plant built on Daihai Lake south shore and lower Eh (the average Eh is-139.27mV) of Daihai Lake result in forming a lot of AVS.
4. The results of speciation analysis, SEM/AVS ratio and a variety of comprehensive assessment show that Cd and Pb in both lake sediments have the highest potential ecological risks and they are priority control pollutants in heavy metal pollution of watery environment.
5. Using three different evaluation method, the evaluation result of heavy metal pollution in the sediments of tow lakes is not consistent. The evaluation results based on the evaluation method of the total amount of heavy metals (except the method of sediment quality criteria) are basically identical, and the sediment pollution level of Daihai Lake is higher than Dalinuoer Lake. Using evaluation method based on forms, the sediment pollution level of Dalinuoer Lake is higher than the Daihai Lake; Using the evaluation method of. SEM/AVS, the results are similar(SEM/AVS in Dalinuoer and Daihai Lake is1.46and1.55respectively). This may be related to the characteristics of evaluation method, the application scope and their limitations. So it is necessary to use a variety of evaluation methods comprehensively in order to complement each other.
本文以中国北方的岱海和达里诺尔为研究对象,以2个湖泊沉积物中重金属的形态分析为基础,系统开展了不同地质背景、不同水质类型湖泊沉积物中重金属赋存形态、AVS与SEM含量及分布特征的对比研究,探讨了重金属在这两个湖泊沉积物中的迁移转化规律,揭示了岱海和达里诺尔湖泊沉积物中重金属形态分布特征与生物有效性的关系,利用基于重金属总量、形态学和ΣSEM/AVS比值法等评价方法,预测和判识了岱海和达里诺尔沉积物中重金属污染可能存在的潜在危害性,得出如下主要结论：
1.研究表明,岱海和达里诺尔湖水质类型分别为氯化物类钠组Ⅰ型水和碳酸盐类钠组Ⅰ型水。2个湖泊矿化度均从上世纪90年代末始逐渐增加,至2011年2个湖泊的氯离子和钠离子均有大幅增长,尤以岱海钙镁比例的失调须引起关注。
2.形态分析表明,铁锰氧化物结合态是岱海沉积物Pb(占总量的43.56%)、Cd(占总量的65.25%)的主导形态,碳酸盐结合态是达里诺尔沉积物Pb(占总量的36.62%)、Cd(占总量的43.89%)的主导形态。总体上,达里诺尔沉积物中Cu、Pb、Zn、Cd的生物有效态含量高于岱海,揭示达里诺尔沉积物中4种重金属的潜在生态风险较高。2个湖泊沉积物中生物有效态重金属的主导形态体现了4种重金属元素的地球化学特性的差异性及2个湖泊水质类型和演化阶段的差异性。
3.研究表明,2个湖泊沉积物中SEM/AVS比值的平均值都大于1,都可能对底栖生物产生毒性作用。尽管岱海硫酸根的含量(170.30mg/L)远小于达里诺尔的硫酸根含量(328.28mg/L),但达里诺尔高盐度(6759.20mg/L)、高碱度(3201.20mg/L)和高pH(9.5)抑制了硫酸盐还原细菌的活性使硫酸根得以保存下来,导致达里诺尔的AVS含量远小于岱海AVS,揭示了达里诺尔沉积物中AVS对重金属的控制作用较弱。此外,岱海南岸建有火力发电厂,其排放的冷却水中含有大量硫酸根离子且岱海水中氧化还原电位较低(平均Eh为-139.27mV),导致大量AVS产生。
4.形态分析、SEM/AVS值及多种综合评价的结果均显示,2个湖泊沉积物中Cd和Pb的潜在生态风险最大,是水环境重金属污染中优先控制的污染物。
5.两个湖泊沉积物中重金属污染用三类评价方法评价的结果并不完全一致,基于重金属总量的评价方法(除沉积物质量基准方法)的评价结果基本一致,且岱海沉积物污染水平高于达里诺尔；基于形态的评价方法中达里诺尔沉积物污染水平高于岱海；而用SEM/AVS的评价结果相近(岱海和达里诺尔沉积物中SEM/AVS分别为1.46、1.55)。这可能与这些评价方法的自身特色、适用范围及其局限性有关,例如基于重金属总量的评价方法的缺点是基准值设定的科学性和合理性有时难以保证。因此,有必要采用多种方法进行综合评价,以便相互补充。
Natural water is a complex multiphase electrolyte system that contains a variety of inorganic and organic matter. AS heavy metals are components of this system, its chemical behavior is necessarily affected by the whole system. Heavy metals pollution in lake sediment is one of the environmental problems facing the world. As one of the widely existing in the nature, heavy metals can be the indicator of water pollution, reflect condition of water-sediment system, while threaten the complex ecosystem of "nature-economy-society" directly or indirectly. So it has important practical significance to recognize the impact of heavy metals on the ecological environment using environmental risk assessment of heavy metals in lake sediment.
The objects of this study are sediments of Daihai Lake and Dalinuoer Lake in northern China. Based on the speciation analysis of heavy metals in both lake sediments, the speciation of heavy metals and the contents and distribution characteristics of AVS and SEM in lake sediment which have different geological background and different types of water quality are compared systematically; the transition and transform rule of heavy metals are discussed in both lake sediments; the relationship between distribution characteristics of speciation and the biological effectiveness of heavy metals in both lake sediments are revealed; being used assessment methods such as the method that is based on the total amount and speciation of heavy metals and∑SEM/AVS ratio, potential hazards of heavy metal pollution in both lake sediments are predicted and sentenced. The major conclusions are as following:
1. The water quality type of Daihai Lake and Dalinuoer Lake is different. The former is I type water of sodium chloride class group, and the latter is I type water of sodium carbonate group. The dissolve solids of both lake have gradually increased since the beginning of the late1990s. Up until2011, the Cl" and Na+of both lake have increased significantly, and the imbalance of Ca/Mg ratio of Daihai Lake especially should be paid close attention.
2. Speciation analysis shows that the dominant speciation of Pb (43.56%of the total) and Cd (65.25%of the total) in the sediments of Daihai Lake is iron and manganese oxides, while the dominant speciation of Pb (36.62%of the total) and Cd (43.89%of the total) in the sediments of Dalinuoer Lake is carbonates. Overall, the bio-available speciation of heavy metals (including Cu,Pb,Zn,Cd) in Dalinuoer Lake sediments is higher than those in Daihai Lake, which reveal that potential ecological risk of those four kinds of heavy metals in Dalinuoer Lake sediments is higher. The dominant speciations of those four kinds of heavy metals in the lakes not only show the difference of the geochemical features among four kinds of heavy metals, but also reveal the difference of lake water quality types and evolution stages between two lakes.
3. Study shows that the average SEM/AVS ratio in both lake sediments are greater than1. So they would have toxic effects on benthos. Although the SO42-concentration (170.30mg/L) of Daihai Lake is far less than Dalinuoer Lake (328.28mg/L), the high salinity (6759.20mg/L), high basicity (3201.20mg/L) and high pH (9.5) of Dalinuoer Lake inhibit the activity of sulfate reducing bacteria so as to make SO4-2be preserved, which leads to the AVS concentration of Dalinuoer Lake is far less than Daihai Lake. This result reveals that the AVS content of Dalinuoer Lake sediments have weak control effects to the heavy metals. In addition, a lot of SO42-in the cooling water discharged by a coal-fired power plant built on Daihai Lake south shore and lower Eh (the average Eh is-139.27mV) of Daihai Lake result in forming a lot of AVS.
4. The results of speciation analysis, SEM/AVS ratio and a variety of comprehensive assessment show that Cd and Pb in both lake sediments have the highest potential ecological risks and they are priority control pollutants in heavy metal pollution of watery environment.
5. Using three different evaluation method, the evaluation result of heavy metal pollution in the sediments of tow lakes is not consistent. The evaluation results based on the evaluation method of the total amount of heavy metals (except the method of sediment quality criteria) are basically identical, and the sediment pollution level of Daihai Lake is higher than Dalinuoer Lake. Using evaluation method based on forms, the sediment pollution level of Dalinuoer Lake is higher than the Daihai Lake; Using the evaluation method of. SEM/AVS, the results are similar(SEM/AVS in Dalinuoer and Daihai Lake is1.46and1.55respectively). This may be related to the characteristics of evaluation method, the application scope and their limitations. So it is necessary to use a variety of evaluation methods comprehensively in order to complement each other.
引文
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