乌梁素海重金属环境地球化学特征及其存在形态数值模拟分析
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摘要
湖泊重金属污染是当今世界上重大的水环境问题，由于其具有生物毒性、生物易富集性及持久性特点，引起了世界各国专家学者的关注，成为学者研究水域与土壤污染的热点。本文以中国北方寒旱区湖泊—乌梁素海为研究对象，综合考虑湖泊整体水环境，分析湖泊水体、沉积物重金属环境地球化学特征，利用地球化学模拟软件（PHREEQC）及地球化学理论知识，对水体中重金属元素存在形态进行分析，并探讨湖泊水环境对重金属赋存形态的影响，主要得出以下结论：
首先对乌梁素海的水环境中重金属的地球化学特征进行了研究分析。将实测的水中重金属数据与国家标准值进行分析比较可知，乌梁素海水体中重金属Cu，Zn，Pb，Cr，Cd，As含量大部分符合地表水水环境III级标准和国家渔业用水标准，重金属Hg含量不符合地表水I级标准和国家渔业用水标准，甚至50%的监测点超出了地表水IV级标准的限定值。选择克里金插值方法对乌梁素海水体中重金属空间分布特征进行分析得知，水体重金属区域分布呈现入水口点源发散状高Hg-Zn-Cr区，出水口条带状高Cu-Pb-Cd-As区，入水口-出水口联片条带状高Cu-As区三个地球化学分区。进一步对水中重金属进行环境评估可知，乌梁素海水中重金属属于轻度污染，湖水致癌风险较低。
其次，为从机理上摸清沉积物中重金属季节性差异的驱动因素，摸清乌梁素海有机化污染、盐化污染、环境特征季节差异大等特点对水环境中重金属迁移转化的影响，对乌梁素海沉积物中重金属的环境地球化学特征进行了研究。系统地分析了乌梁素海沉积物中重金属在冬季与夏季的变化特征及污染程度，并考虑乌梁素海特殊的水环境特征，结合多种环境条件研究影响重金属季节变化的因素进行分析得知，乌梁素海沉积物重金属Cu，Zn，Pb，Cr，Cd污染具有相似特征，均已受到不同程度污染，主要表现为冬季大于夏季；重金属Hg，As污染较严重，主要表现为夏季大于冬季。温度、水动力条件、有机质含量与粒度属于Cu，Zn，Pb，Cr和Cd季节分布特征主控因子；氧化还原条件和盐度属于Hg和As的主控因子。采用基于因子分析的主成分方法分析了乌梁素海重金属的主要来源，主要为自然风化和沉积、工业污染以及农业面源污染与大气沉降。在分析沉积物季节变化特征与污染源的基础上，通过改进BCR逐级提取法对重金属形态分析并结合沉积物理化性质、水环境因素的变化特征，系统探讨了影响重金属化学形态与生物活性的因素，并从重金属形态学角度对沉积物重金属状况进行评估，分析结果显示：1）重金属总量对残渣态影响较大，2）pH对酸可提取态、有机物和硫化物结合态影响较大，3）有机质与酸可提取态，有机物和硫化物结合态有较大相关性，4）盐度与酸可提取态、有机物和硫化物结合态有一定的相关性，5）总氮，总磷与有机物和硫化物结合态有一定的相关性，6）乌梁素海重金属Cd是生物活性最强、污染最严重的金属，Hg污染次之，应该对Cd与Hg给予特别关注。
在对水环境中重金属环境地球化学特征分析的基础上，对水体中重金属元素存在形态进行了进一步的模拟研究。利用HSC Chemistry v5.0软件以及物理化学理论，新建了Hg，Cr，As这三种重金属元素的存在形态模拟数据库，并且对重金属Cu，Zn，Pb，Cd在原有数据库的基础上进行了补充。利用地球化学模拟软件以及环境地球化学的理论知识研究湖泊水体中重金属的存在形态，分析重金属元素在湖泊水体中毒性最小的存在状态与存在环境，模拟结果分析可知，乌梁素海湖泊水体中七种重金属元素主要以CuCl_2~-、CuCl_3~(2-)、CuCO_3、Cu(OH)_2、Zn~(2+)、Zn(OH)_2、ZnCO_3、ZnSO_4、PbCO_3、PbOH~+、Pb(CO_3)_2~(2-)、Cr(OH)_3、Cr(OH)_2~+、CdCl~+、Cd~(2+)、CdSO_4、CdCl_2、Hg(OH)_2、HgCl_3~-、HgCl_2、HAsO_4~(2-)及H3AsO_3为优势态。在目前水环境现状下重金属形态分析的基础上，考虑乌梁素海环境特征季节差异大的特点，利用PHREEQC软件进行模拟，分析水体温度、氧化还原性、酸碱性的改变对重金属元素存在形态的影响，结果表明：1）温度对七种重金属的各种存在形态最终分布无大影响。2）水体中七种重金属重金属的存在形态受pH影响较大，水体pH较低时，重金属主要以配合反应为主，此时水体中Cl-，SO_4~(2-)等阴离子配位体含量对其影响较为明显；随着pH的升高，重金属逐渐发生水解反应。3）水体的氧化还原性对不同重金属有不同影响。当水体处于还原状态时，水体中重金属Cu主要以CuCl_2~-含量最大，As主要以H3AsO_3和H2AsO_3-占主导地位；处于氧化性状态时，Cu(OH)_2含量最大，HAsO_4~(2-)和H2AsO_4-占主导地位。在水体处于弱碱性-中性状态前提下，氧化还原电位发生变化并不会对水体中重金属Cr的形态有较大影响。重金属Hg、Zn、Pb、Cd、Cr的存在形态并不会随着氧化还原电位变化而发生改变。
最后，根据本文的研究结果及湖泊重金属防治的经验，最终提出了对乌梁素海重金属的治理的几点对策与建议：1）控制外源污染源排放。结合重金属污染来源，控制工业污废水的排放，加快污水处理厂建设；禁止使用含汞、砷及镉等重金属的农药化肥，并通过合理的施肥，减少化肥的流失；控制大气汞的排放；2）控制内源重金属污染物负荷。在摸清乌梁素海重金属元素在湖泊沉积物中的赋存形态及影响因素的前提下，控制水环境条件、沉积物理化性质等外界条件抑制重金属释放，从而达到降低重金属污染风险的目的；3）以摸清乌梁素海重金属元素在湖泊水体中的各种存在形态为基础进行重金属的污染治理，控制各种外界环境条件，选择合适的方法降低重金属元素的污染风险。
The heavy metal pollution in lakes is a serious problem, which has been payinggrowing attention because of their toxicity and subsequent accumulation in aquatichabitats. This paper studied the speciation and the environmental geochemicalcharacteristics of seven heavy metals including mercury (Hg), zinc (Zn), chromium (Cr),copper (Cu), lead (Pb), cadmium (Cd), and arsenic (As) in water and sediment inWuliangsuhai Lake (WL) of Inner Mongolia. The pollution sources were analyzed byPrincipal component analysis method and the speciation of these metals and the factorsimpacting their existing status were analyzed by PHREEQC model. The main findingsare listed as below:
Firstly, environmental geochemistry of heavy metal of WL is studied and analyzed.The water quality data combined with national standard value are analyzed. For themetals of Cu, Zn, Pb, Cr, Cd, and As, most of the samples collected for the seven metalsmeet the national surface water quality standard first level and the national fisherystandard。The pollution of Hg did not meet the national surface water quality standard Iand the national fishery standard, and50%of the samples did not meet the surface waterquality standard IV. The spatial estimate and analysis on variability of heavy metal areanalyzed by Kriging. It shows the spatial distribution of the heavy metals with highconcentrations can be classified as the point pattern of Hg-Zn-Cr at the inlet of the lake,the strip pattern of Cu-Pb-Cd-As at the outlet, and the strip pattern of Cu-As at both inletand outlet. The environmental pollution is analyzed using the method of IntegratedPollution Index and the health risk model. The water heavy metal pollution of WL isslightly and the carcinogen risk level is low.
In order to explain the driving factors for seasonal difference, selected sediment datato research environmental geochemistry of sediments. Based on the geoaccumulationindex, i) Cu, Zn, Pb, Cr, and Cd were more polluted in winter than in summer; ii) Hg andAs were more polluted in summer than in winter. Based on the correlation analysis,temperature, hydrodynamic conditions, organic matter concentration, and particle sizewere the main control factors for seasonal distribution pattern and Hg and As were themain control factors for redox and salinity properties. Principal component analysis(PCA) was used to identify the different pollutant sources. The results demonstrated that the heavy metal sources are the parent rocks, industrial pollution, agriculturalnon-point-source pollution and atmospheric deposition. The chemical speciation of Cu,Zn, Pb, Cr, Cd, Hg, and As in sediment was analyzed based on the EuropeanCommunities Bureau of Reference (BCR) fractionation method. The correlation of thechemical speciation and biological activity among these metals were analyzed based ontheir chemical and physical characteristics, and the ratio of secondary phase to primaryphase (KRSP) was employed to assess the heavy metal pollution in sediments.The resultsshow that i) total concentration is the most important factor affecting the residual fraction;ii) organic matter, pH, and salinity are the primary factors affecting the acid extractabilityand the adsorption of sulfur compound by organic matter; iii) total nitrogen and totalphosphorus are the main factors affecting the adsorption of sulfur compound on organicmatter. Iiii) based on the total concentration and bioavailability, Cd is the most risk metal,followed by Hg. So, more attention should be paid to Cd and Hg pollution in WL.
As different chemical species in water have different toxity to organism, thespeciation of the studied metals in WL was analyzed with the PHREEQC model. TheHREEQC database for these heavy metals was established with HSC Chemistry v5.0software. The chemical species of Hg, Cr, As, Cu, Zn, Pb and Cd in water solution werefound from literature. The results indicate that CuCl_2~-, CuCl_3~(2-), CuCO_3, Cu(OH)_2, Zn~(2+),Zn (OH)_2, ZnCO_3, ZnSO_4, PbCO_3, PbOH~+, Pb(CO_3)_2~(2-), Cr(OH)_3, Cr(OH)_2~+, CdCl~+, Cd~(2+),CdSO_4, CdCl_2, Hg(OH)_2, HgCl_3~-, HgCl_2, HAsO_4~(2-), and H3AsO_3are the dominant speciesin WL. As HgCl_2is very toxic and mercury pollution did not meet the national standard,Hg pollution should be paid more attention. With the change of seasonal weather, thetemperature, redox, and pH of the lake will be changed. The impact of temperature, redoxand pH on the heavy metal species in WL was simulated with the PHREEQC software.The results are as follow: i) the change of temperature have minor impact on thespeciation of this heavy metals.ii) pH influences greatly the speciation of these heavymetals. In the condition of low pH, the counter hydrolysis reaction of heavy metals isdominant, which is intermediated by Cl-and SO_4~(2-)ions. In the condition of high pH, thehydrolysis reaction of heavy metals is dominant. iii) Water redox condition in the lakehas different effects on heavy metal speciation. In the reduction condition, CuCl_2~-,H3AsO_3, and H2AsO_3-are the dominant species for Cu and As metals. In the oxidationcondition, Cu(OH)_2, HAsO_4~(2-), and H2AsO_4-are dominant species. At the weak alkalinestate, redox potential change has minor impact on Cr speciation. Hg, Zn, Pb, Cd, and Crspecies do not change while the redox condition changes in lake.
At last, based on the findings of this study, the following suggestions to control WL pollution are provided; i) The toxity of the studied heavy metals depends on thespeciation in water solution, which can be controlled by the external environmentalconditions, such as pH, redox of the lake; ii) The external pollutant emitted from industryshould be controlled;3) The internal pollutant from sediment should be controlled byreducing disturbance to the bed of WL.
首先对乌梁素海的水环境中重金属的地球化学特征进行了研究分析。将实测的水中重金属数据与国家标准值进行分析比较可知，乌梁素海水体中重金属Cu，Zn，Pb，Cr，Cd，As含量大部分符合地表水水环境III级标准和国家渔业用水标准，重金属Hg含量不符合地表水I级标准和国家渔业用水标准，甚至50%的监测点超出了地表水IV级标准的限定值。选择克里金插值方法对乌梁素海水体中重金属空间分布特征进行分析得知，水体重金属区域分布呈现入水口点源发散状高Hg-Zn-Cr区，出水口条带状高Cu-Pb-Cd-As区，入水口-出水口联片条带状高Cu-As区三个地球化学分区。进一步对水中重金属进行环境评估可知，乌梁素海水中重金属属于轻度污染，湖水致癌风险较低。
其次，为从机理上摸清沉积物中重金属季节性差异的驱动因素，摸清乌梁素海有机化污染、盐化污染、环境特征季节差异大等特点对水环境中重金属迁移转化的影响，对乌梁素海沉积物中重金属的环境地球化学特征进行了研究。系统地分析了乌梁素海沉积物中重金属在冬季与夏季的变化特征及污染程度，并考虑乌梁素海特殊的水环境特征，结合多种环境条件研究影响重金属季节变化的因素进行分析得知，乌梁素海沉积物重金属Cu，Zn，Pb，Cr，Cd污染具有相似特征，均已受到不同程度污染，主要表现为冬季大于夏季；重金属Hg，As污染较严重，主要表现为夏季大于冬季。温度、水动力条件、有机质含量与粒度属于Cu，Zn，Pb，Cr和Cd季节分布特征主控因子；氧化还原条件和盐度属于Hg和As的主控因子。采用基于因子分析的主成分方法分析了乌梁素海重金属的主要来源，主要为自然风化和沉积、工业污染以及农业面源污染与大气沉降。在分析沉积物季节变化特征与污染源的基础上，通过改进BCR逐级提取法对重金属形态分析并结合沉积物理化性质、水环境因素的变化特征，系统探讨了影响重金属化学形态与生物活性的因素，并从重金属形态学角度对沉积物重金属状况进行评估，分析结果显示：1）重金属总量对残渣态影响较大，2）pH对酸可提取态、有机物和硫化物结合态影响较大，3）有机质与酸可提取态，有机物和硫化物结合态有较大相关性，4）盐度与酸可提取态、有机物和硫化物结合态有一定的相关性，5）总氮，总磷与有机物和硫化物结合态有一定的相关性，6）乌梁素海重金属Cd是生物活性最强、污染最严重的金属，Hg污染次之，应该对Cd与Hg给予特别关注。
在对水环境中重金属环境地球化学特征分析的基础上，对水体中重金属元素存在形态进行了进一步的模拟研究。利用HSC Chemistry v5.0软件以及物理化学理论，新建了Hg，Cr，As这三种重金属元素的存在形态模拟数据库，并且对重金属Cu，Zn，Pb，Cd在原有数据库的基础上进行了补充。利用地球化学模拟软件以及环境地球化学的理论知识研究湖泊水体中重金属的存在形态，分析重金属元素在湖泊水体中毒性最小的存在状态与存在环境，模拟结果分析可知，乌梁素海湖泊水体中七种重金属元素主要以CuCl_2~-、CuCl_3~(2-)、CuCO_3、Cu(OH)_2、Zn~(2+)、Zn(OH)_2、ZnCO_3、ZnSO_4、PbCO_3、PbOH~+、Pb(CO_3)_2~(2-)、Cr(OH)_3、Cr(OH)_2~+、CdCl~+、Cd~(2+)、CdSO_4、CdCl_2、Hg(OH)_2、HgCl_3~-、HgCl_2、HAsO_4~(2-)及H3AsO_3为优势态。在目前水环境现状下重金属形态分析的基础上，考虑乌梁素海环境特征季节差异大的特点，利用PHREEQC软件进行模拟，分析水体温度、氧化还原性、酸碱性的改变对重金属元素存在形态的影响，结果表明：1）温度对七种重金属的各种存在形态最终分布无大影响。2）水体中七种重金属重金属的存在形态受pH影响较大，水体pH较低时，重金属主要以配合反应为主，此时水体中Cl-，SO_4~(2-)等阴离子配位体含量对其影响较为明显；随着pH的升高，重金属逐渐发生水解反应。3）水体的氧化还原性对不同重金属有不同影响。当水体处于还原状态时，水体中重金属Cu主要以CuCl_2~-含量最大，As主要以H3AsO_3和H2AsO_3-占主导地位；处于氧化性状态时，Cu(OH)_2含量最大，HAsO_4~(2-)和H2AsO_4-占主导地位。在水体处于弱碱性-中性状态前提下，氧化还原电位发生变化并不会对水体中重金属Cr的形态有较大影响。重金属Hg、Zn、Pb、Cd、Cr的存在形态并不会随着氧化还原电位变化而发生改变。
最后，根据本文的研究结果及湖泊重金属防治的经验，最终提出了对乌梁素海重金属的治理的几点对策与建议：1）控制外源污染源排放。结合重金属污染来源，控制工业污废水的排放，加快污水处理厂建设；禁止使用含汞、砷及镉等重金属的农药化肥，并通过合理的施肥，减少化肥的流失；控制大气汞的排放；2）控制内源重金属污染物负荷。在摸清乌梁素海重金属元素在湖泊沉积物中的赋存形态及影响因素的前提下，控制水环境条件、沉积物理化性质等外界条件抑制重金属释放，从而达到降低重金属污染风险的目的；3）以摸清乌梁素海重金属元素在湖泊水体中的各种存在形态为基础进行重金属的污染治理，控制各种外界环境条件，选择合适的方法降低重金属元素的污染风险。
The heavy metal pollution in lakes is a serious problem, which has been payinggrowing attention because of their toxicity and subsequent accumulation in aquatichabitats. This paper studied the speciation and the environmental geochemicalcharacteristics of seven heavy metals including mercury (Hg), zinc (Zn), chromium (Cr),copper (Cu), lead (Pb), cadmium (Cd), and arsenic (As) in water and sediment inWuliangsuhai Lake (WL) of Inner Mongolia. The pollution sources were analyzed byPrincipal component analysis method and the speciation of these metals and the factorsimpacting their existing status were analyzed by PHREEQC model. The main findingsare listed as below:
Firstly, environmental geochemistry of heavy metal of WL is studied and analyzed.The water quality data combined with national standard value are analyzed. For themetals of Cu, Zn, Pb, Cr, Cd, and As, most of the samples collected for the seven metalsmeet the national surface water quality standard first level and the national fisherystandard。The pollution of Hg did not meet the national surface water quality standard Iand the national fishery standard, and50%of the samples did not meet the surface waterquality standard IV. The spatial estimate and analysis on variability of heavy metal areanalyzed by Kriging. It shows the spatial distribution of the heavy metals with highconcentrations can be classified as the point pattern of Hg-Zn-Cr at the inlet of the lake,the strip pattern of Cu-Pb-Cd-As at the outlet, and the strip pattern of Cu-As at both inletand outlet. The environmental pollution is analyzed using the method of IntegratedPollution Index and the health risk model. The water heavy metal pollution of WL isslightly and the carcinogen risk level is low.
In order to explain the driving factors for seasonal difference, selected sediment datato research environmental geochemistry of sediments. Based on the geoaccumulationindex, i) Cu, Zn, Pb, Cr, and Cd were more polluted in winter than in summer; ii) Hg andAs were more polluted in summer than in winter. Based on the correlation analysis,temperature, hydrodynamic conditions, organic matter concentration, and particle sizewere the main control factors for seasonal distribution pattern and Hg and As were themain control factors for redox and salinity properties. Principal component analysis(PCA) was used to identify the different pollutant sources. The results demonstrated that the heavy metal sources are the parent rocks, industrial pollution, agriculturalnon-point-source pollution and atmospheric deposition. The chemical speciation of Cu,Zn, Pb, Cr, Cd, Hg, and As in sediment was analyzed based on the EuropeanCommunities Bureau of Reference (BCR) fractionation method. The correlation of thechemical speciation and biological activity among these metals were analyzed based ontheir chemical and physical characteristics, and the ratio of secondary phase to primaryphase (KRSP) was employed to assess the heavy metal pollution in sediments.The resultsshow that i) total concentration is the most important factor affecting the residual fraction;ii) organic matter, pH, and salinity are the primary factors affecting the acid extractabilityand the adsorption of sulfur compound by organic matter; iii) total nitrogen and totalphosphorus are the main factors affecting the adsorption of sulfur compound on organicmatter. Iiii) based on the total concentration and bioavailability, Cd is the most risk metal,followed by Hg. So, more attention should be paid to Cd and Hg pollution in WL.
As different chemical species in water have different toxity to organism, thespeciation of the studied metals in WL was analyzed with the PHREEQC model. TheHREEQC database for these heavy metals was established with HSC Chemistry v5.0software. The chemical species of Hg, Cr, As, Cu, Zn, Pb and Cd in water solution werefound from literature. The results indicate that CuCl_2~-, CuCl_3~(2-), CuCO_3, Cu(OH)_2, Zn~(2+),Zn (OH)_2, ZnCO_3, ZnSO_4, PbCO_3, PbOH~+, Pb(CO_3)_2~(2-), Cr(OH)_3, Cr(OH)_2~+, CdCl~+, Cd~(2+),CdSO_4, CdCl_2, Hg(OH)_2, HgCl_3~-, HgCl_2, HAsO_4~(2-), and H3AsO_3are the dominant speciesin WL. As HgCl_2is very toxic and mercury pollution did not meet the national standard,Hg pollution should be paid more attention. With the change of seasonal weather, thetemperature, redox, and pH of the lake will be changed. The impact of temperature, redoxand pH on the heavy metal species in WL was simulated with the PHREEQC software.The results are as follow: i) the change of temperature have minor impact on thespeciation of this heavy metals.ii) pH influences greatly the speciation of these heavymetals. In the condition of low pH, the counter hydrolysis reaction of heavy metals isdominant, which is intermediated by Cl-and SO_4~(2-)ions. In the condition of high pH, thehydrolysis reaction of heavy metals is dominant. iii) Water redox condition in the lakehas different effects on heavy metal speciation. In the reduction condition, CuCl_2~-,H3AsO_3, and H2AsO_3-are the dominant species for Cu and As metals. In the oxidationcondition, Cu(OH)_2, HAsO_4~(2-), and H2AsO_4-are dominant species. At the weak alkalinestate, redox potential change has minor impact on Cr speciation. Hg, Zn, Pb, Cd, and Crspecies do not change while the redox condition changes in lake.
At last, based on the findings of this study, the following suggestions to control WL pollution are provided; i) The toxity of the studied heavy metals depends on thespeciation in water solution, which can be controlled by the external environmentalconditions, such as pH, redox of the lake; ii) The external pollutant emitted from industryshould be controlled;3) The internal pollutant from sediment should be controlled byreducing disturbance to the bed of WL.
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