土对重金属离子的吸附解吸特性及其迁移修复机制研究
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摘要
重金属污染土非常普遍,危害性大,有必要开展重金属离子在典型土中的归宿、迁移特性与修复的研究。本文以室内试验为基础,系统分析了多种因素(离子浓度、pH、温度、土水比等)影响下四种重金属离子(Cd、Cu、Pb、Zn)在两种典型土(高岭土和Q_4黄土)中的吸附、解吸特性及其机理;提出了一套基于质量浓度的运移参数反演新方法;新定义了基于解吸过程的解吸附分配系数,相应提出了解吸等温线的分析方法;发展了可模拟污染土修复过程的试验方法与理论模型,获得了一系列有意义的结论。
1)重金属离子在土壤上的吸附受离子类型、土质、平衡时间、pH、土水比的共同影响;黄土中方解石成分对Pb(Ⅱ)、Cu(Ⅱ)的吸附具有重要贡献,而对Zn(Ⅱ)、Cd(Ⅱ)的吸附作用甚微;首次发现黄土中粉质石英可吸附Pb(Ⅱ)、Cd(Ⅱ)、Zn(Ⅱ);高岭石、针铁矿等粘土矿物会产生表面络合型吸附。
2)试验验证并表征了解吸滞回特性和络合物在土中再吸附的现象,发现其与离子类型、离子的初始浓度、土壤质地、解吸方法等密切相关。提出的基于解吸过程的解吸附分配系数可考虑离子初始浓度和解吸方法,优于现有方法。
3)建立了基于土中污染物总质量浓度的运移参数反演新方法,并编制了反分析程序;通过对已有文献数据及本文土柱试验结果的整理分析验证了所提方法的合理性,此方法具有概念清晰、测试简便、结果稳定的特点。
4)一维土柱扩散试验表明黄土阻滞Pb(Ⅱ)、Cd(Ⅱ)的能力明显优于高岭土,污染物在土中的有效扩散系数随离子半径增加而减小:Pb(Ⅱ)＜Cd(Ⅱ)＜Zn(Ⅱ);土柱法反演所得的K_d明显小于Batch法的结果;建议用土柱法测定运移参数。
5)采用衰变型运移理并对络合物运移过程进行简化,建立了可模拟修复过程的理论模型,并在试验结果分析中得到验证;土柱解吸试验表明络合剂NTA可极大提高冲洗法对重金属污染土的修复能力,且对Cd(Ⅱ)的解吸效果好于Pb(Ⅱ),对污染高岭土的修复效果明显好于黄土,有望应用于污染场地的冲洗法修复之中。
Widely distributed soil pollution by heavy metals requires studies of fate and transport of heavy metals in typical soils in China. This dissertation is designated to investigate the adsorption/desorption behavior and mechanism of four heavy metals (Cd, Cu, Pb, Zn) on two typical soils (Kaolin and Q_4 Loess) on the basis of laboratory experiments. Several factors (i.e. ionic strength, pH, temperature, solid solution ratio etc.) have been studied with regarding their effects on adsorption/desorption characteristics and the relevant mechanisms. A novel parameterization method was put forward to calculate the transport parameters (partitioning coefficient and effective diffusion coefficient). A novel desorption partitioning coefficient was defined along with a novel parameterization method. Novel analysis scheme and the theoretical model were both developed to simulate the remediation of heavy metals polluted soil using a comlexing agent. A series of significant conclusions were drawn accordingly.
1) The adsorption of heavy metals on soils is controlled by ion type, soil constituent, equilibrating duration, pH, solid solution ratio etc. The calcite in loess was found greatly responsible for adsorption of Pb(II) and Cu(II) instead of Zn(II) and Cd(II). The silty quartz in loess was found for the first time responsible for adsorption of Pb(II), Cd(II), Zn(II). Kaolinite can react with heavy metals in the form of surface complexes to give rise to the adsorption capacity of soils.
2) The hysterisis behavior of desorption from soils and the re-adsorption of heavy metal complexes on soil components were experimentally verified and theoretically characterised. The desorption behavior of four metal cations from Kaolin and loess were systematically investigated and found correlated with ion type, initial ion concentration, soil component and desorption method etc. The proposed desorption-process-oriented desorption partition coefficient could take into account of solute concentration and desorption method and thus appeared superior to the convetional definition.
3) A new method was established and incoporated into a compiled code to parameterize the transport of pollutant in soil on the basis of total mass concentrations. The proposed method was testified by analyzing both the reported data and test results in this study. This method was characterized with clear concepts, convenient handling and stable results.
4) Diffusion behavior of heavy metals in one dimensional soil column was studied by experiments. The parameterized method was verified and some improvement was made. The inhibiting Pb(II) and Cd(II) diffusion ability of loess was found better than kaolin. The effective diffusion coefficient of metal ions in soil columns became smaller along with the increasing radius of metal ions: Pb(II) 5) A theoretical model (decaying transport theory and complexing simplification) was put forward and was experimentally verified reasonable to simulate the remediation of polluted soil. Column leaching tests showed that the complexing agent NTA can greatly improve the remedying performance of heavy metals polluted soil. NTA could remove more Cd than Pb from polluted soil, and could remove more pollutant from kaolin than from loess, and thus appears applicable in pump-and-treatment remediation of contaminated sites.
1)重金属离子在土壤上的吸附受离子类型、土质、平衡时间、pH、土水比的共同影响;黄土中方解石成分对Pb(Ⅱ)、Cu(Ⅱ)的吸附具有重要贡献,而对Zn(Ⅱ)、Cd(Ⅱ)的吸附作用甚微;首次发现黄土中粉质石英可吸附Pb(Ⅱ)、Cd(Ⅱ)、Zn(Ⅱ);高岭石、针铁矿等粘土矿物会产生表面络合型吸附。
2)试验验证并表征了解吸滞回特性和络合物在土中再吸附的现象,发现其与离子类型、离子的初始浓度、土壤质地、解吸方法等密切相关。提出的基于解吸过程的解吸附分配系数可考虑离子初始浓度和解吸方法,优于现有方法。
3)建立了基于土中污染物总质量浓度的运移参数反演新方法,并编制了反分析程序;通过对已有文献数据及本文土柱试验结果的整理分析验证了所提方法的合理性,此方法具有概念清晰、测试简便、结果稳定的特点。
4)一维土柱扩散试验表明黄土阻滞Pb(Ⅱ)、Cd(Ⅱ)的能力明显优于高岭土,污染物在土中的有效扩散系数随离子半径增加而减小:Pb(Ⅱ)＜Cd(Ⅱ)＜Zn(Ⅱ);土柱法反演所得的K_d明显小于Batch法的结果;建议用土柱法测定运移参数。
5)采用衰变型运移理并对络合物运移过程进行简化,建立了可模拟修复过程的理论模型,并在试验结果分析中得到验证;土柱解吸试验表明络合剂NTA可极大提高冲洗法对重金属污染土的修复能力,且对Cd(Ⅱ)的解吸效果好于Pb(Ⅱ),对污染高岭土的修复效果明显好于黄土,有望应用于污染场地的冲洗法修复之中。
Widely distributed soil pollution by heavy metals requires studies of fate and transport of heavy metals in typical soils in China. This dissertation is designated to investigate the adsorption/desorption behavior and mechanism of four heavy metals (Cd, Cu, Pb, Zn) on two typical soils (Kaolin and Q_4 Loess) on the basis of laboratory experiments. Several factors (i.e. ionic strength, pH, temperature, solid solution ratio etc.) have been studied with regarding their effects on adsorption/desorption characteristics and the relevant mechanisms. A novel parameterization method was put forward to calculate the transport parameters (partitioning coefficient and effective diffusion coefficient). A novel desorption partitioning coefficient was defined along with a novel parameterization method. Novel analysis scheme and the theoretical model were both developed to simulate the remediation of heavy metals polluted soil using a comlexing agent. A series of significant conclusions were drawn accordingly.
1) The adsorption of heavy metals on soils is controlled by ion type, soil constituent, equilibrating duration, pH, solid solution ratio etc. The calcite in loess was found greatly responsible for adsorption of Pb(II) and Cu(II) instead of Zn(II) and Cd(II). The silty quartz in loess was found for the first time responsible for adsorption of Pb(II), Cd(II), Zn(II). Kaolinite can react with heavy metals in the form of surface complexes to give rise to the adsorption capacity of soils.
2) The hysterisis behavior of desorption from soils and the re-adsorption of heavy metal complexes on soil components were experimentally verified and theoretically characterised. The desorption behavior of four metal cations from Kaolin and loess were systematically investigated and found correlated with ion type, initial ion concentration, soil component and desorption method etc. The proposed desorption-process-oriented desorption partition coefficient could take into account of solute concentration and desorption method and thus appeared superior to the convetional definition.
3) A new method was established and incoporated into a compiled code to parameterize the transport of pollutant in soil on the basis of total mass concentrations. The proposed method was testified by analyzing both the reported data and test results in this study. This method was characterized with clear concepts, convenient handling and stable results.
4) Diffusion behavior of heavy metals in one dimensional soil column was studied by experiments. The parameterized method was verified and some improvement was made. The inhibiting Pb(II) and Cd(II) diffusion ability of loess was found better than kaolin. The effective diffusion coefficient of metal ions in soil columns became smaller along with the increasing radius of metal ions: Pb(II)
引文
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