挥发性氯代烃在我国典型土壤中的吸附—解吸特性研究
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摘要
近年来,中国土壤污染事故频发,引起了社会和政府部门的广泛关注。吸附是挥发性氯代烃(Volatile chlorinated hydrocarbons,VCHs)污染土壤的主要机制之一。土壤对VCHs的吸附行为不仅直接影响土壤中VCHs的浓度及其分布,而且影响VCHs在土壤中的迁移转化,并对污染现场的修复能力产生重大影响。因此,了解VCHs在土壤中的吸附特性对于污染场地调查与修复有着重要的实际意义。在对VCHs在土壤中的吸附-解吸行为进行调研的基础上,本研究定量解析了我国典型土壤与常见VCHs气体的吸附平衡关系,建立了根据土壤气体浓度预测土壤中污染物含有量的方法,同时用连续通气实验研究了四氯乙烯(tetrachloroethylene, PCE)从长期污染土壤中的解吸特性,为推进我国调查和控制城市地区的土壤污染提供理论基础。主要包括以下3部分内容:
(1)采用静态吸附平衡实验测试3类干燥水稻土对6种VCHs气体的吸附平衡。结果显示干燥土壤的平衡吸附等温线用Dubinin-Astakhov方程拟合良好(R2>0.95),且方程参数与土壤和VCHs特性的有关。Dubinin-Astakhov等式各参数不受土壤有机碳含量的影响;β与VCHs化合物的分子体积之间没有发现相关性,但随VCHs分子极性的增大有变大的趋势;E0与土壤的V<平均孔径呈线性相关;W_0与V_(<10nm)相关良好,但与土壤比表面积关系不大。用Dubinin-Astakhov方程进行干燥土壤的平衡吸附量预测,预测值与实测值拟合良好(R~2=0.98)。
(2)用动态吸附平衡实验测试8类湿润土壤对4种VCHs气体的吸附平衡。发现湿润土壤对三氯乙烯、四氯乙烯、1,1,1-三氯乙烷的吸附等温线符合Henry型吸附等温式,而1,1,2-三氯乙烷则呈非线性吸附。不同土壤的固-液吸附平衡系数(KSW)与土壤有机碳含量(α)呈良好的线性关系。对湿润土壤的平衡吸附量进行预测,预测值与实测值相关良好(R~2=0.98)。对于含水率介于干燥与湿润之间的半湿润土壤的吸附不能忽略直接暴露于气相中的水合土壤表面的吸附,这部分与干燥土壤有类似的吸附机制,可以通过压汞法和BET N_2吸附法得到暴露于气相中的土壤表面比例γ和土壤的相对饱和度RS。这样,半湿润土壤的吸附量可以用干燥和湿润土壤的预测式进行估算。
(3)用连续通气实验解析PCE从长期污染土壤中的解吸特性。脱离气体中PCE浓度随通气时间而降低,特别是在通气初期一段时间里浓度急剧下降。通气过程中的PCE去除率与污染土壤的粒径分布和有机碳含量有关。通气结束后,有一部分PCE难以通气脱离,这是因为吸附于土壤有机碳、矿物晶体内及粒子层间的PCE扩散缓慢的缘故。
In recent years, soil pollution accidents had happened frequently in China, and had aroused wide attention of government and community. Adsorption is one of the principal mechanisms of soil contamination by volatile chlorinated hydrocarbons (VCHs). The adsorption behaviors of VCHs onto soil not only directly affect the concentration of VCHs and distribution in soil, but also influence the VCHs migration and transformation in soil, and also have a significant impact on the ability of remediation of contaminated site. Therefore, understanding the adsorption characteristics of VCHs onto soil has important practical significance for the investigation and remediation of contaminated sites. On the basis of reviewing the adsorption-desorption behaviors onto soils, the adsorption equilibrium relationships between VCHs gases and typical soils in China were quantitatively analyzed and methods used to predict quantity of pollutants in soil according to soil gas concentrations was established in this study. Besides, the desorption behavior of tetrachloroethylene (PCE) from long-term contaminated soils was studied using continuous air stripping. Thus, provide a theoretical basis for promoting the investigation and control of soil pollution in urban areas. The study mainly includes the following three parts:
(1)The equilibrium adsorption of 6 VCHs gases onto 3 dry paddy soils was studied using static equilibrium adsorption experiments. Results showed that the equilibrium adsorption isotherms of dry soils could be well fitted with the Dubinin-Astakhov equation (R~2>0.95). Parameters of the Dubinin-Astakhov equation were influenced by the characteristics of soils and VCHs. No correlation was found between the parameters and soil organic carbon content. The affinity coefficients (β) did not show significant dependence on the molecular volumes of VCHs but tended to increase along with the increase in the molecular polarities. The adsorption energies (E_0) of the reference compound (tetrachloroethylene) positively correlated to the pore volume with radius below the average (V (2)The equilibrium adsorption of 4 VCHs gases onto 8 moist soils were studied using dynamic equilibrium experiments. It was found that adsorption isotherms of trichloroethylene, tetrachloroethylene, 1,1,1-trichloroethane, could be described by Henry equation, but the adsorption isotherms of 1,1,2-trichloroethane was non-linear. The soil-water adsorption equilibrium coefficients KSW showed a good linear relationship with soils’organic carbon content (α). The adsorbed amounts of wet soils agreed well with the measured values (R2=0.98). For soils with water content between dry and moist soils, the adsorption onto the hydrated soil surface exposed directly to the vapor phase which was similar to dry soil can’t be neglected. The relative saturation of soil (RS) and the fraction of soil surface exposed to the vapor phase (γ) can be obtained by combining mercury intrusion data and BET adsorption data. Thus, the adsorbed amounts by those soils can be estimated using the predicted equations of dry and moist soils.
(3)Continuous ventilation experiment was conducted to study the desorption behavior from unsaturated soils which were long-term contaminated by PCE. The PCE concentration in the effluent air decreased with time of ventilation, mostly during the early stages of air injection. The PCE removal rate was related to the soil particle size distribution and soil organic carbon content. Some fraction of adsorbed PCE couldn’t be removed at the end of ventilation, because the process of diffusion from soil was difficult due to the strong adsorption in soil organic carbon, crystallization of minerals and porous particle layers.
(1)采用静态吸附平衡实验测试3类干燥水稻土对6种VCHs气体的吸附平衡。结果显示干燥土壤的平衡吸附等温线用Dubinin-Astakhov方程拟合良好(R2>0.95),且方程参数与土壤和VCHs特性的有关。Dubinin-Astakhov等式各参数不受土壤有机碳含量的影响;β与VCHs化合物的分子体积之间没有发现相关性,但随VCHs分子极性的增大有变大的趋势;E0与土壤的V<平均孔径呈线性相关;W_0与V_(<10nm)相关良好,但与土壤比表面积关系不大。用Dubinin-Astakhov方程进行干燥土壤的平衡吸附量预测,预测值与实测值拟合良好(R~2=0.98)。
(2)用动态吸附平衡实验测试8类湿润土壤对4种VCHs气体的吸附平衡。发现湿润土壤对三氯乙烯、四氯乙烯、1,1,1-三氯乙烷的吸附等温线符合Henry型吸附等温式,而1,1,2-三氯乙烷则呈非线性吸附。不同土壤的固-液吸附平衡系数(KSW)与土壤有机碳含量(α)呈良好的线性关系。对湿润土壤的平衡吸附量进行预测,预测值与实测值相关良好(R~2=0.98)。对于含水率介于干燥与湿润之间的半湿润土壤的吸附不能忽略直接暴露于气相中的水合土壤表面的吸附,这部分与干燥土壤有类似的吸附机制,可以通过压汞法和BET N_2吸附法得到暴露于气相中的土壤表面比例γ和土壤的相对饱和度RS。这样,半湿润土壤的吸附量可以用干燥和湿润土壤的预测式进行估算。
(3)用连续通气实验解析PCE从长期污染土壤中的解吸特性。脱离气体中PCE浓度随通气时间而降低,特别是在通气初期一段时间里浓度急剧下降。通气过程中的PCE去除率与污染土壤的粒径分布和有机碳含量有关。通气结束后,有一部分PCE难以通气脱离,这是因为吸附于土壤有机碳、矿物晶体内及粒子层间的PCE扩散缓慢的缘故。
In recent years, soil pollution accidents had happened frequently in China, and had aroused wide attention of government and community. Adsorption is one of the principal mechanisms of soil contamination by volatile chlorinated hydrocarbons (VCHs). The adsorption behaviors of VCHs onto soil not only directly affect the concentration of VCHs and distribution in soil, but also influence the VCHs migration and transformation in soil, and also have a significant impact on the ability of remediation of contaminated site. Therefore, understanding the adsorption characteristics of VCHs onto soil has important practical significance for the investigation and remediation of contaminated sites. On the basis of reviewing the adsorption-desorption behaviors onto soils, the adsorption equilibrium relationships between VCHs gases and typical soils in China were quantitatively analyzed and methods used to predict quantity of pollutants in soil according to soil gas concentrations was established in this study. Besides, the desorption behavior of tetrachloroethylene (PCE) from long-term contaminated soils was studied using continuous air stripping. Thus, provide a theoretical basis for promoting the investigation and control of soil pollution in urban areas. The study mainly includes the following three parts:
(1)The equilibrium adsorption of 6 VCHs gases onto 3 dry paddy soils was studied using static equilibrium adsorption experiments. Results showed that the equilibrium adsorption isotherms of dry soils could be well fitted with the Dubinin-Astakhov equation (R~2>0.95). Parameters of the Dubinin-Astakhov equation were influenced by the characteristics of soils and VCHs. No correlation was found between the parameters and soil organic carbon content. The affinity coefficients (β) did not show significant dependence on the molecular volumes of VCHs but tended to increase along with the increase in the molecular polarities. The adsorption energies (E_0) of the reference compound (tetrachloroethylene) positively correlated to the pore volume with radius below the average (V
(3)Continuous ventilation experiment was conducted to study the desorption behavior from unsaturated soils which were long-term contaminated by PCE. The PCE concentration in the effluent air decreased with time of ventilation, mostly during the early stages of air injection. The PCE removal rate was related to the soil particle size distribution and soil organic carbon content. Some fraction of adsorbed PCE couldn’t be removed at the end of ventilation, because the process of diffusion from soil was difficult due to the strong adsorption in soil organic carbon, crystallization of minerals and porous particle layers.
引文
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