太湖溶解性有机质对Cu的形态及生物有效性的影响
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摘要
重金属在水环境中积累引起的潜在危害不仅对我们的环境带来了威胁，也对人体健康产生了威胁。通常，重金属的生物有效性与水环境的物理化学条件有关系，其中溶解性有机质（Dissolved organic matter, DOM）是控制天然水环境中的重金属的生物地球化学行为和毒性的重要因素之一。重金属在太湖的污染也越来越引起了人们的关注，本文在国家973计划项目“湖泊水环境质量演变与水环境基准研究”（2008CB418201）子课题“湖泊水环境质量区域差异特征”和江苏省研究生培养创新工程项目“太湖DOM对重金属在沉积物-水相中分配的影响”（CXZZ11-0317）资助下，完成了全太湖的上覆水、孔隙水和沉积物等200多个样品进行了调查、取样和测试分析，获得有效数据30000多个。在野外调查的基础上，开展了室内模拟实验，并利用实验结果建立了模型，系统探讨了太湖DOM对Cu的形态及生物有效性的影响。研究成果将为由中国环境保护部提出的中国的环境基准战略提供基础数据，为建立适用于我国生态和经济形势的水环境基准体系提供科学支持。本研究的主要结论有以下几点：
（1）野外测试结果表明，上覆水中，重金属浓度在太湖水体中的含量通常都不高，无论是CCC值（基准连续浓度值,又称为慢性基准值）还是CMC值（基准最大浓度值，又称为急性基准值）都不会给生态环境带来风险。孔隙水中，大多数重金属浓度的含量要低于上覆水中的含量。但是在沉积物中，与当地土壤背景值相比较，重金属都表现出富集现象。空间分布上，无论是上覆水还是沉积物中，大多数重金属从漕桥河到湖泊都表现出一个明显的浓度梯度，这反应了入湖河流对太湖的影响。通过分析沉积物中重金属形态发现：重金属潜在的生物有效性部分含量占到重金属总量的8.4%(Cr)到55.6%(Cu)，Cu对水生生物的毒性风险最大。统计显示，太湖沉积物中有机质比起pH值对重金属分布和形态的影响作用更为显著。
（2）吸附-解吸实验表明，难溶性有机质可以将更多的Cu从水相中吸附到沉积物中，而DOM则增加了沉积物的吸附容量。通过定量化分析太湖不同湖区沉积物中DOM对Cu的潜在结合容量发现，包含较多腐殖质物质外源有机质比湖泊内源有机质对Cu具有更高的结合容量。三维荧光光谱结果表明DOM中腐殖质对Cu的结合容量从11.5mg/g到151.4mg/g，而类蛋白物质的结合容量为26.3mg/g到35.4mg/g。根据DOM结合容量和太湖DOM含量计算可得，如果太湖水体中Cu的含量低于7.87mg/l，Cu将全部以DOM结合态的形式存在于水体中。解析实验表明，沉积物中难溶性有机质可以与Cu形成稳定的化合物，而DOM则有利于Cu的迁移。
（3）平衡渗透实验结果表明，太湖南部湖区DOM分子量主要为>3500Da的有机物，而北部湖区DOM的分子量范围则为<10000Da。总体上看，南部湖区DOM的分子量要高于北部湖区DOM的分子量。通过分析不同分子量DOM中的物质发现，高分子量的DOM主要为腐殖酸物质，而低分子量的DOM则主要为类蛋白物质。离子选择性电极结果和光谱学结果表明Cu倾向于被太湖低分子量的DOM结合。
（4）降解实验表明，太湖水体DOM可以在紫外光照射下显著降解，DOM在72h到168h之间降解速度的最快。紫外波长和3DEEM结果表明：在紫外光照条件下，a254的值和四类荧光峰迅速降低，表明DOM被完全降解。而在避光条件下，a254和A254/A400值表明微生物作用可以将大分子的DOM降解为小分子的DOM。DOM中各种组分在不同降解条件下的差异性可以对DOM和Cu的相互作用产生不同效果。在紫外光照条件下，Cu的存在可以促进DOM的降解，而在避光条件下，Cu却抑制了微生物对DOM的降解作用。
（5）DOM浓度和化学组成极大的地影响着Cu的化学形态，进而影响着Cu的生物有效性和水质基准值。根据太湖DOM的浓度范围和HA在DOM中的百分比含量范围，以及对太湖水环境质量调查结果，生物配体模型（BLM）被用来预测太湖中Cu的形态、生物有效性和水环境质量基准值。结果表明DOM浓度和组成极大的影响着Cu的形态，进而影响着Cu的生物有效性和水质基准值。随着DOM浓度的增加和HA在DOM中百分比含量的增加，Cu对大型蚤的急性毒性值和水质基准值都呈线性关系增长。
Potential danger raised by metal accumulation in aquatic environments and inaquatic organisms not only poses threat to our environments but also to the food safety.Generally, bioavailability of heavy metals is related to physical and chemicalconditions of the aquatic environment. In particular，the dissolved organic matters isimportant control over the biogeochemical behavior and toxicity of heavy metals innatural waters. The heavy metal pollution in the Taihu Lake has been becoming moreand more serious. So we studied the influence of DOM in Taihu Lake on the speciesand bioavailability of Cu, and this work will provide a data base for the ongoingChina’s criteria strategy, which proposed recently by the Ministry of EnvironmentProtection of China to establish its own water quality criteria system based on China’secological and economic situation. Main contents of the thesis are listed as follows:
(1) Metal concentrations in the water column in Taihu Lake were generally lowand would not give rise to ecological risks either for the CCC or CMC values. Theconcentration of most metals in the interstitial water was not higher than in the watercolumn. In the sediment, metals were enriched compared with the background valuesfor local soil. Spatially, many metals presented a clear spatial gradient in both watercolumn and sediment from the Caoqiao River to the lake, which is a reflection of theimpact of river input s to the lake. The potential bio-available fraction of the heavymetals accounted for8.4%(Cr) to55.6%(Cu) of the total metal concentration.Statistical analysis indicated that organic matters had a significantly stronger controlon the metal distribution and species than pH in Taihu sediment.
(2) Insoluble organic matter of sediment can absorb most Cu from water phaseand DOM could greatly enhance the sorption capacity. Through quantitativelycharacterizes the Cu binding potential of DOM in sediment from different part ofTaihu Lake, results show that the exogenous DOM included more humic matters thanendogenous DOM and had higher complex capacity than Taihu Lake DOM. Thefluorescence quenching results reflect that the complex capacity of humic componentsin DOM was from111.5mg/g to151.4mg/g, however, the complex capacity of proteincomponents was from26.3mg/g to35.4mg/g. According to the complex capacity andDOM concentration in Taihu Lake, it was calculated that if the Cu concentration inTaihu Lake water was less than7.87mg/l, Cu would exist as DOM complexation inthe water column. The desorption experiment indicated that insoluble organic matters could form the most stable complexes, however, DOM was favorable for the metaltransportation.（3）The equilibrium membrane dialysis method was employed to determine themolecular weight distribution of dissolved organic matters in the Taihu Lake sediment.Results indicate that Taihu DOM was dominated with the molecular weight>3500Dain south lake, while DOM was dominated with the molecular weight between<10000Da. Overall, south lake DOM had a higher molecular weight than that in northlake. Through analyzing the substances in different molecular weight DOM, it wasfound that the high molecular weight DOM was mainly consisted by the humicmatters while the low molecular weight DOM was mainly comprised by theprotein-lake matters. The ISE results and3DEEM spectral characteristics showed thatCu tended to be associated with low molecular weight DOM in Taihu Lake.
(4) DOM in the Taihu water was significantly degraded under UV radiation. Theconcentration of TOC declined quickly between72h and168h. UV absorption and3DEEM results showed that the a254decreased quickly and the four fluorescencepeaks also disappeared quickly under UV radiation condition. This indicated a morecomplete degradation under UV radiation. Under the dark condition, the a254andA254/A400ratio showed the action of microorganisms in converting high molecularweight substances into low molecular weight substances. The Variation of degradationbehavior of different components in DOM can caused different effects on theinteraction between DOM and Cu. Under UV condition，Cu can promote thedegradation of DOM by the UV radiation, however, in dark， Cu inhibit thedegradation of DOM by microbes.
(5) According the range of DOM concentration and percentage of HA in DOM,BLM was used to predict the species, bio-available and Water quality criteria of Cubased on the investigation of Taihu Lake water quality. The results indicated that theDOM concentration and components significantly influenced the species of Cu andthen influenced the bio-available and water quality criteria of Cu. With the increase ofDOM concentration or the percentage of HA, acute toxicity and water quality criteriaof Cu to Daphnia magna increased with a linear correlation.
（1）野外测试结果表明，上覆水中，重金属浓度在太湖水体中的含量通常都不高，无论是CCC值（基准连续浓度值,又称为慢性基准值）还是CMC值（基准最大浓度值，又称为急性基准值）都不会给生态环境带来风险。孔隙水中，大多数重金属浓度的含量要低于上覆水中的含量。但是在沉积物中，与当地土壤背景值相比较，重金属都表现出富集现象。空间分布上，无论是上覆水还是沉积物中，大多数重金属从漕桥河到湖泊都表现出一个明显的浓度梯度，这反应了入湖河流对太湖的影响。通过分析沉积物中重金属形态发现：重金属潜在的生物有效性部分含量占到重金属总量的8.4%(Cr)到55.6%(Cu)，Cu对水生生物的毒性风险最大。统计显示，太湖沉积物中有机质比起pH值对重金属分布和形态的影响作用更为显著。
（2）吸附-解吸实验表明，难溶性有机质可以将更多的Cu从水相中吸附到沉积物中，而DOM则增加了沉积物的吸附容量。通过定量化分析太湖不同湖区沉积物中DOM对Cu的潜在结合容量发现，包含较多腐殖质物质外源有机质比湖泊内源有机质对Cu具有更高的结合容量。三维荧光光谱结果表明DOM中腐殖质对Cu的结合容量从11.5mg/g到151.4mg/g，而类蛋白物质的结合容量为26.3mg/g到35.4mg/g。根据DOM结合容量和太湖DOM含量计算可得，如果太湖水体中Cu的含量低于7.87mg/l，Cu将全部以DOM结合态的形式存在于水体中。解析实验表明，沉积物中难溶性有机质可以与Cu形成稳定的化合物，而DOM则有利于Cu的迁移。
（3）平衡渗透实验结果表明，太湖南部湖区DOM分子量主要为>3500Da的有机物，而北部湖区DOM的分子量范围则为<10000Da。总体上看，南部湖区DOM的分子量要高于北部湖区DOM的分子量。通过分析不同分子量DOM中的物质发现，高分子量的DOM主要为腐殖酸物质，而低分子量的DOM则主要为类蛋白物质。离子选择性电极结果和光谱学结果表明Cu倾向于被太湖低分子量的DOM结合。
（4）降解实验表明，太湖水体DOM可以在紫外光照射下显著降解，DOM在72h到168h之间降解速度的最快。紫外波长和3DEEM结果表明：在紫外光照条件下，a254的值和四类荧光峰迅速降低，表明DOM被完全降解。而在避光条件下，a254和A254/A400值表明微生物作用可以将大分子的DOM降解为小分子的DOM。DOM中各种组分在不同降解条件下的差异性可以对DOM和Cu的相互作用产生不同效果。在紫外光照条件下，Cu的存在可以促进DOM的降解，而在避光条件下，Cu却抑制了微生物对DOM的降解作用。
（5）DOM浓度和化学组成极大的地影响着Cu的化学形态，进而影响着Cu的生物有效性和水质基准值。根据太湖DOM的浓度范围和HA在DOM中的百分比含量范围，以及对太湖水环境质量调查结果，生物配体模型（BLM）被用来预测太湖中Cu的形态、生物有效性和水环境质量基准值。结果表明DOM浓度和组成极大的影响着Cu的形态，进而影响着Cu的生物有效性和水质基准值。随着DOM浓度的增加和HA在DOM中百分比含量的增加，Cu对大型蚤的急性毒性值和水质基准值都呈线性关系增长。
Potential danger raised by metal accumulation in aquatic environments and inaquatic organisms not only poses threat to our environments but also to the food safety.Generally, bioavailability of heavy metals is related to physical and chemicalconditions of the aquatic environment. In particular，the dissolved organic matters isimportant control over the biogeochemical behavior and toxicity of heavy metals innatural waters. The heavy metal pollution in the Taihu Lake has been becoming moreand more serious. So we studied the influence of DOM in Taihu Lake on the speciesand bioavailability of Cu, and this work will provide a data base for the ongoingChina’s criteria strategy, which proposed recently by the Ministry of EnvironmentProtection of China to establish its own water quality criteria system based on China’secological and economic situation. Main contents of the thesis are listed as follows:
(1) Metal concentrations in the water column in Taihu Lake were generally lowand would not give rise to ecological risks either for the CCC or CMC values. Theconcentration of most metals in the interstitial water was not higher than in the watercolumn. In the sediment, metals were enriched compared with the background valuesfor local soil. Spatially, many metals presented a clear spatial gradient in both watercolumn and sediment from the Caoqiao River to the lake, which is a reflection of theimpact of river input s to the lake. The potential bio-available fraction of the heavymetals accounted for8.4%(Cr) to55.6%(Cu) of the total metal concentration.Statistical analysis indicated that organic matters had a significantly stronger controlon the metal distribution and species than pH in Taihu sediment.
(2) Insoluble organic matter of sediment can absorb most Cu from water phaseand DOM could greatly enhance the sorption capacity. Through quantitativelycharacterizes the Cu binding potential of DOM in sediment from different part ofTaihu Lake, results show that the exogenous DOM included more humic matters thanendogenous DOM and had higher complex capacity than Taihu Lake DOM. Thefluorescence quenching results reflect that the complex capacity of humic componentsin DOM was from111.5mg/g to151.4mg/g, however, the complex capacity of proteincomponents was from26.3mg/g to35.4mg/g. According to the complex capacity andDOM concentration in Taihu Lake, it was calculated that if the Cu concentration inTaihu Lake water was less than7.87mg/l, Cu would exist as DOM complexation inthe water column. The desorption experiment indicated that insoluble organic matters could form the most stable complexes, however, DOM was favorable for the metaltransportation.（3）The equilibrium membrane dialysis method was employed to determine themolecular weight distribution of dissolved organic matters in the Taihu Lake sediment.Results indicate that Taihu DOM was dominated with the molecular weight>3500Dain south lake, while DOM was dominated with the molecular weight between<10000Da. Overall, south lake DOM had a higher molecular weight than that in northlake. Through analyzing the substances in different molecular weight DOM, it wasfound that the high molecular weight DOM was mainly consisted by the humicmatters while the low molecular weight DOM was mainly comprised by theprotein-lake matters. The ISE results and3DEEM spectral characteristics showed thatCu tended to be associated with low molecular weight DOM in Taihu Lake.
(4) DOM in the Taihu water was significantly degraded under UV radiation. Theconcentration of TOC declined quickly between72h and168h. UV absorption and3DEEM results showed that the a254decreased quickly and the four fluorescencepeaks also disappeared quickly under UV radiation condition. This indicated a morecomplete degradation under UV radiation. Under the dark condition, the a254andA254/A400ratio showed the action of microorganisms in converting high molecularweight substances into low molecular weight substances. The Variation of degradationbehavior of different components in DOM can caused different effects on theinteraction between DOM and Cu. Under UV condition，Cu can promote thedegradation of DOM by the UV radiation, however, in dark， Cu inhibit thedegradation of DOM by microbes.
(5) According the range of DOM concentration and percentage of HA in DOM,BLM was used to predict the species, bio-available and Water quality criteria of Cubased on the investigation of Taihu Lake water quality. The results indicated that theDOM concentration and components significantly influenced the species of Cu andthen influenced the bio-available and water quality criteria of Cu. With the increase ofDOM concentration or the percentage of HA, acute toxicity and water quality criteriaof Cu to Daphnia magna increased with a linear correlation.
引文
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