重金属污染物在红壤中迁移规律及修复技术研究
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摘要
土壤是组成地球生态环境的重要部分，也是人类生存的宝贵资源。近年来，随着采矿业、冶金业、铸造业以及电子业的迅猛发展，土壤重金属污染状况日益严重。在过去50年里，粗略统计排放到全球环境中的镉达到2.2×104吨、铜9.39×105吨、铅7.83×105吨、锌1.35×106吨。其中有相当一部分进入土壤，致使世界各国土壤出现不同程度的污染问题。土壤重金属污染致使人类生存环境质量恶化，导致各类污染事件频发，严重危害生态系统的良性循环和人类的生存健康。因而，土壤重金属污染修复技术成为研究热点。
目前各国都在为研究与开发重金属污染土壤修复技术作出努力，常规的重金属污染土壤修复技术有物理修复技术、化学修复技术、植物修复技术、微生物修复技术以及电动力学修复技术等。但以上土壤修复技术存在运行费用高、片面强调土壤污染而忽视了土壤——地下水系统的整体性、对环境造成二次污染、可操作性差等局限性，因而能够工程化的土壤修复技术十分有限。
针对以上问题，本课题以我国南昌地区特征土壤——红壤作为研究对象，以铜和镍为特征污染物，提出新的土壤修复技术——可降解螯合剂淋洗法+可渗透反应格栅（chelating agent-permeable reactive barrier，CH-PRB）治理土壤重金属污染。淋洗法是传统的土壤修复技术，国内外的环境工作者已具备完善的工程经验。可渗透反应格栅（permeable reactive barrier，PRB）技术是一种新的地下水处理技术，该技术在国外已有广泛应用。CH-PRB土壤修复技术将土壤和地下水视为整体，在修复重金属污染土壤的同时，处理受污染的地下水。且CH-PRB技术采用经筛选的、可生物降解螯合剂作为淋洗剂，在保证土壤中重金属物质去除效果的同时，避免了对环境造成的二次污染。
本课题通过人工模拟污染红壤，进行重金属（铜和镍）在红壤中赋存形态特征研究。研究证明：在铜污染红壤中铜的赋存形态以可交换态为主，占总含铜量的31.98%；在镍污染红壤中镍的赋存形态以可残渣态为主，占总含镍量的57.49%，其次才是可交换态，占总含镍量的29.53%。
搭建直径为30cm，高200cm的土柱试验，以硫酸铜溶液为特征污染物，以浅层积水，自由漫流进水形式向土柱持续注入硫酸铜溶液，模拟硫酸铜溶液在红壤中的扩散过程，研究重金属在红壤中的扩散、赋存形态的分布及迁移规律，并运用瞬间剖面法计算出重金属溶液在红壤中的水动力弥散系数，建立重金属污染物在埋深小于100cm土层中水动力弥散系数分布方程。以对流——弥散模型(Convective——Dispersive Model，CD模型)为基础，耦合水动力弥散系数分布方程，建立了土壤表面存在重金属溶液浅层积水条件下，红壤中重金属溶质迁移模型。
通过烧杯试验，对比研究壳聚糖、EDTA及柠檬酸三钠三种螯合剂对红壤中重金属（铜和镍）的浸提效果。研究表明，生物螯合剂——壳聚糖可作为淋洗液应用于修复红壤的重金属污染，且多种重金属共存时，在浸提过程中各种金属间表现出明显的协同作用。
构建CH-PRB土壤修复技术系统，以0.2g/L壳聚糖溶液作为淋洗液对直径20cm，高100cm，平均含铜量为2.34mg/g铜污染土柱进行修复试验。修复进行42天，待修复土壤中铜的去除率达到98.29%，土壤中残存的重金属铜含量仅为0.04mg/g，低于《土壤环境质量标准》（GB15618-1995）中规定的二级土壤含铜量最高限值——0.05mg/g。为了高效去除土壤淋洗渗出液及地下水中存在的重金属污染物质，本课题采用平行对比试验，对可渗透反应格栅中的填料材料进行筛选。研究证明，废铁屑+活性炭+粉煤渣按照1:1:1体积比混合，作为CH-PRB土壤修复技术中可渗透反应格栅的填料，可对土壤淋洗渗出液及地下水中的重金属和有机物起到很好的去除效果。最终出水水质为：[Cu]=0mg/L，COD=9.80mg/L，pH值=5.11-5.12。研究结果证明CH-PRB土壤修复技术可高效、稳定、持续处理红壤及地下水中重金属污染物质。
参照连续搅拌反应器（CSTR），建立可降解螯合剂淋洗系统的反应动力学模型，确立了污染土壤体积、土壤中重金属提取率与淋洗液停留时间、淋洗时间等因素之间的关系，初步构建了CH-PRB土壤修复技术的设计体系，为该技术的推广与应用提供参考。
Soil is an important part of ecological environment, and is one of the main resources which humanbeings must depend upon for survival. In the recent years, the heavy metal pollution of soil hasincreased with the development of mining industry, metallurgical industry, foundry industry andelectronic industry. According to statistics, in the past50years, the emission amount of cadmium was2.2×104tons, copper was9.39×105tons, lead was7.83×105tons, and zinc was1.35×106tons. Aconsiderable portion of those heavy metals had been absorbed into the system of soil and undergroundwater, which caused heavy metal pollutions in the world. That means the heavy metal pollution has ledto deterioration of soil quality, and caused frequent heavy metal contaminations in human society. Theheavy metal pollution of soil has been a threat to the circulation of soil ecosystem and the human beingsurvival. Therefore, the heavy metal remediation technology has become a research hotspot.
The physical technology, the chemical technology, the phytoremediation technology, the microbialremediation technology and the electro-chemical technology are the traditional technologies to restorethe soil heavy metal contaminnation. Although the researchers are working for developing the heavymetal remediation technology, those remediation technologies still have some problems, such as, thehigh operating cost, the pollution of underground water, the secondary pollution to the environment,and the feasibility. So few technologies can be applied in engineerings.
According to the drawbacks, the new soil remediation technology—CH-PRB (biodegradable chelatingagent+permeable reactive barrier) was raised in the project. In this project, the red soil was the object of thestudy, and the copper and the nickel were the specific pollutants. Leaching method is the traditional soilremediation technology and the researchers have enough engineering experiences on it. The technology ofPRB (permeable reactive barrier) is a new groundwater treatment technology, which has been widely used inforeign countries. The two techniques are combined in the CH-PRB technology, which is able to restore thesoil and the polluted groundwater which contaminated by heavy metal at the same time. And thegreen-chelating agents are used in the CH-PRB technology as the eluents to remove the heavy metal in thesoil, while avoiding secondary pollution in the environment.
The study of the copper and nickel speciations in the artificial-contaminated soil were performed toevaluate the heavy metals distribution in the red soil. The analyzed results have indicated: the exchangeablefraction of copper was the high proportion in the copper-contaminated soil, which was31.98%, while inthe nickel-contaminated soil the most portion was observed in the residual form, up to57.49%, and theexchangeable fraction was29.53%.
Conducting the soil column experiment(diameter was20cm, height was100cm), with the solution ofCuSO4slowly filting down into the soil column simulating the diffusion of copper in the red soil, themigration regularity of copper in the red soil was studied and the hydrodynamic diffusion coefficient in thedifferent layers were calculated using the instantaneous profile method. Basing the advection dispersion model and using the finite-difference time-domain method, the heavy metal migration model wasestablished, which coupled with the hydrodynamic diffusion coefficient.
By the beaker test, with the copper and the nickel were the specific pollutants, the heavy metalsextraction efficiencies of chitosan, ethylene diamine citric acid, and sodium citrate from the red soilwere compared in the project. The studies have shown that the biological chelating agent-chitosancould be used as the eluent in the leaching process to remediate the heavy metal contaminated red soil,and the coexistence of a variety of heavy metals would make the heavy metals show good synergisticproperties in the process of extraction.
With the model of the soil remediation process of CH-PRB, the contaminated soil columnexperiment, which diameter was20cm, height was100cm, and copper content was2.340mg/g, wasstudied. Using the0.2g/L chitosan solution as the eluent, the removal efficieny of the tested soil columnwas98.29%, and the remaining copper content in the soil was only0.04mg/g, which was lower thanthe upper limit of copper content in the second class soil in Environmental Quality Standards for Soils(GB15618-1995). By parallel experiments, the results have shown that the reaction filler which wasconsisted of the iron scrap, activated carbon powder, and cinder with the volume rate of1:1:1, was themost effective matter filled in the permeable reactive barrier. This kind of reaction filler could removethe heavy metal in the exudates of the contaminated soil column and in the underground water. Thefinal influent with [Cu]=0mg/L, COD=9.80mg/L, pH=5.11-5.12was obtained. The studies havedemonstrated that the soil remediation process of CH-PRB could restore the heavy metal contaminatedred soil efficiently and steadily, and this process was sustainable.
Referring to the continuous stirred tank reactor (CSTR), the reaction kinetics model of thebiodegradable chelating agent leaching system in the CH-PRB was established. Furthermore, therelation between the extraction efficiency of the heavy metal, the volume of contaminated soil and theresidence time of eluent, the leaching time were discussed. At the same time, the initial construction ofthe CH-PRB soil remediation process design system was set up, which will offer references for theapplication of this new process.
目前各国都在为研究与开发重金属污染土壤修复技术作出努力，常规的重金属污染土壤修复技术有物理修复技术、化学修复技术、植物修复技术、微生物修复技术以及电动力学修复技术等。但以上土壤修复技术存在运行费用高、片面强调土壤污染而忽视了土壤——地下水系统的整体性、对环境造成二次污染、可操作性差等局限性，因而能够工程化的土壤修复技术十分有限。
针对以上问题，本课题以我国南昌地区特征土壤——红壤作为研究对象，以铜和镍为特征污染物，提出新的土壤修复技术——可降解螯合剂淋洗法+可渗透反应格栅（chelating agent-permeable reactive barrier，CH-PRB）治理土壤重金属污染。淋洗法是传统的土壤修复技术，国内外的环境工作者已具备完善的工程经验。可渗透反应格栅（permeable reactive barrier，PRB）技术是一种新的地下水处理技术，该技术在国外已有广泛应用。CH-PRB土壤修复技术将土壤和地下水视为整体，在修复重金属污染土壤的同时，处理受污染的地下水。且CH-PRB技术采用经筛选的、可生物降解螯合剂作为淋洗剂，在保证土壤中重金属物质去除效果的同时，避免了对环境造成的二次污染。
本课题通过人工模拟污染红壤，进行重金属（铜和镍）在红壤中赋存形态特征研究。研究证明：在铜污染红壤中铜的赋存形态以可交换态为主，占总含铜量的31.98%；在镍污染红壤中镍的赋存形态以可残渣态为主，占总含镍量的57.49%，其次才是可交换态，占总含镍量的29.53%。
搭建直径为30cm，高200cm的土柱试验，以硫酸铜溶液为特征污染物，以浅层积水，自由漫流进水形式向土柱持续注入硫酸铜溶液，模拟硫酸铜溶液在红壤中的扩散过程，研究重金属在红壤中的扩散、赋存形态的分布及迁移规律，并运用瞬间剖面法计算出重金属溶液在红壤中的水动力弥散系数，建立重金属污染物在埋深小于100cm土层中水动力弥散系数分布方程。以对流——弥散模型(Convective——Dispersive Model，CD模型)为基础，耦合水动力弥散系数分布方程，建立了土壤表面存在重金属溶液浅层积水条件下，红壤中重金属溶质迁移模型。
通过烧杯试验，对比研究壳聚糖、EDTA及柠檬酸三钠三种螯合剂对红壤中重金属（铜和镍）的浸提效果。研究表明，生物螯合剂——壳聚糖可作为淋洗液应用于修复红壤的重金属污染，且多种重金属共存时，在浸提过程中各种金属间表现出明显的协同作用。
构建CH-PRB土壤修复技术系统，以0.2g/L壳聚糖溶液作为淋洗液对直径20cm，高100cm，平均含铜量为2.34mg/g铜污染土柱进行修复试验。修复进行42天，待修复土壤中铜的去除率达到98.29%，土壤中残存的重金属铜含量仅为0.04mg/g，低于《土壤环境质量标准》（GB15618-1995）中规定的二级土壤含铜量最高限值——0.05mg/g。为了高效去除土壤淋洗渗出液及地下水中存在的重金属污染物质，本课题采用平行对比试验，对可渗透反应格栅中的填料材料进行筛选。研究证明，废铁屑+活性炭+粉煤渣按照1:1:1体积比混合，作为CH-PRB土壤修复技术中可渗透反应格栅的填料，可对土壤淋洗渗出液及地下水中的重金属和有机物起到很好的去除效果。最终出水水质为：[Cu]=0mg/L，COD=9.80mg/L，pH值=5.11-5.12。研究结果证明CH-PRB土壤修复技术可高效、稳定、持续处理红壤及地下水中重金属污染物质。
参照连续搅拌反应器（CSTR），建立可降解螯合剂淋洗系统的反应动力学模型，确立了污染土壤体积、土壤中重金属提取率与淋洗液停留时间、淋洗时间等因素之间的关系，初步构建了CH-PRB土壤修复技术的设计体系，为该技术的推广与应用提供参考。
Soil is an important part of ecological environment, and is one of the main resources which humanbeings must depend upon for survival. In the recent years, the heavy metal pollution of soil hasincreased with the development of mining industry, metallurgical industry, foundry industry andelectronic industry. According to statistics, in the past50years, the emission amount of cadmium was2.2×104tons, copper was9.39×105tons, lead was7.83×105tons, and zinc was1.35×106tons. Aconsiderable portion of those heavy metals had been absorbed into the system of soil and undergroundwater, which caused heavy metal pollutions in the world. That means the heavy metal pollution has ledto deterioration of soil quality, and caused frequent heavy metal contaminations in human society. Theheavy metal pollution of soil has been a threat to the circulation of soil ecosystem and the human beingsurvival. Therefore, the heavy metal remediation technology has become a research hotspot.
The physical technology, the chemical technology, the phytoremediation technology, the microbialremediation technology and the electro-chemical technology are the traditional technologies to restorethe soil heavy metal contaminnation. Although the researchers are working for developing the heavymetal remediation technology, those remediation technologies still have some problems, such as, thehigh operating cost, the pollution of underground water, the secondary pollution to the environment,and the feasibility. So few technologies can be applied in engineerings.
According to the drawbacks, the new soil remediation technology—CH-PRB (biodegradable chelatingagent+permeable reactive barrier) was raised in the project. In this project, the red soil was the object of thestudy, and the copper and the nickel were the specific pollutants. Leaching method is the traditional soilremediation technology and the researchers have enough engineering experiences on it. The technology ofPRB (permeable reactive barrier) is a new groundwater treatment technology, which has been widely used inforeign countries. The two techniques are combined in the CH-PRB technology, which is able to restore thesoil and the polluted groundwater which contaminated by heavy metal at the same time. And thegreen-chelating agents are used in the CH-PRB technology as the eluents to remove the heavy metal in thesoil, while avoiding secondary pollution in the environment.
The study of the copper and nickel speciations in the artificial-contaminated soil were performed toevaluate the heavy metals distribution in the red soil. The analyzed results have indicated: the exchangeablefraction of copper was the high proportion in the copper-contaminated soil, which was31.98%, while inthe nickel-contaminated soil the most portion was observed in the residual form, up to57.49%, and theexchangeable fraction was29.53%.
Conducting the soil column experiment(diameter was20cm, height was100cm), with the solution ofCuSO4slowly filting down into the soil column simulating the diffusion of copper in the red soil, themigration regularity of copper in the red soil was studied and the hydrodynamic diffusion coefficient in thedifferent layers were calculated using the instantaneous profile method. Basing the advection dispersion model and using the finite-difference time-domain method, the heavy metal migration model wasestablished, which coupled with the hydrodynamic diffusion coefficient.
By the beaker test, with the copper and the nickel were the specific pollutants, the heavy metalsextraction efficiencies of chitosan, ethylene diamine citric acid, and sodium citrate from the red soilwere compared in the project. The studies have shown that the biological chelating agent-chitosancould be used as the eluent in the leaching process to remediate the heavy metal contaminated red soil,and the coexistence of a variety of heavy metals would make the heavy metals show good synergisticproperties in the process of extraction.
With the model of the soil remediation process of CH-PRB, the contaminated soil columnexperiment, which diameter was20cm, height was100cm, and copper content was2.340mg/g, wasstudied. Using the0.2g/L chitosan solution as the eluent, the removal efficieny of the tested soil columnwas98.29%, and the remaining copper content in the soil was only0.04mg/g, which was lower thanthe upper limit of copper content in the second class soil in Environmental Quality Standards for Soils(GB15618-1995). By parallel experiments, the results have shown that the reaction filler which wasconsisted of the iron scrap, activated carbon powder, and cinder with the volume rate of1:1:1, was themost effective matter filled in the permeable reactive barrier. This kind of reaction filler could removethe heavy metal in the exudates of the contaminated soil column and in the underground water. Thefinal influent with [Cu]=0mg/L, COD=9.80mg/L, pH=5.11-5.12was obtained. The studies havedemonstrated that the soil remediation process of CH-PRB could restore the heavy metal contaminatedred soil efficiently and steadily, and this process was sustainable.
Referring to the continuous stirred tank reactor (CSTR), the reaction kinetics model of thebiodegradable chelating agent leaching system in the CH-PRB was established. Furthermore, therelation between the extraction efficiency of the heavy metal, the volume of contaminated soil and theresidence time of eluent, the leaching time were discussed. At the same time, the initial construction ofthe CH-PRB soil remediation process design system was set up, which will offer references for theapplication of this new process.
引文
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