不同初始氧化还原电位土壤中重金属Cd/Zn/Cu的运移实验及数值模拟
摘要
土壤化学环境是人类生活的重要环境因素之一,重金属污染物能通过多种途径进入土壤并不断富集,从而影响着土壤的化学环境。由于土壤对重金属离子的强吸附性,传统上把土壤中的重金属看作是不动的,但是当土壤环境发生变化时,重金属离子就会释放到土壤溶液中,并随之运移到地下水中,对地下水环境造成污染。氧化还原反应是土壤中一种基本的化学和生物化学过程,可通过改变离子的价态而对土壤中无机物和有机物的存在形态、吸附、迁移转化等过程产生作用。因此研究土壤的氧化还原电位对重金属迁移转化的影响,对深入了解重金属在土壤中的运移行为和归宿、评价其污染风险以及进行污染修复有重要意义。
本文以较为常见的镉、锌、铜三种重金属作为研究对象,以五种不同初始氧化还原电位(Eh)的土壤为介质,首先研究了静态情况下,三种重金属的吸附、竞争吸附特性；接着重点研究了三种重金属在五种不同初始Eh土壤中的迁移规律,并进一步探讨了多种重金属共存时,竞争吸附作用对其迁移规律和作用机理的影响,并应用美国盐土实验室研制的HYDRUS-1D软件,模拟了重金属在土壤中的穿透曲线,获得了拟合参数；最后运用这些参数对土壤不同埋深条件下重金属的迁移行为进行预测。得出以下结论：
1)在静态等温吸附实验中,五种不同初始Eh土壤对单一重金属离子的吸附量存在很大差别,还原性土壤>原棕壤>氧化性土壤；随着平衡液中重金属浓度的增加,土壤对重金属的吸附量呈增大趋势。当两种重金属共存时,土壤对单一重金属的吸附量要大于两种重金属共存时的吸附量；三种重金属离子共存时,重金属离子的竞争吸附能力大小顺序为：Cu2+>Cd2+>Zn2+。另外,随着平衡液中重金属浓度的增大,平衡液的pH呈下降趋势,Eh呈现上升趋势且均高于土壤初始Eh,平衡液的电导率(Ec)呈上升趋势,且氧化性土壤的Ec大于还原性土壤的Ec。用Langmuir方程和Freundlich方程对数据进行拟合,确定性系数R2都在0.948以上,总体拟合效果较好,Freundlich方程的拟合效果更佳。
2)Br-在棕壤中迁移的穿透曲线(BTCs)具有较好的对称性,说明土壤的物理非平衡影响较小。与Br-的BTCs相比,不同初始Eh土壤对三种重金属BTCs的形状和峰值等都有影响,所有能检测出重金属的BTCs均呈现出不同程度的非对称性,解吸部分有较长的“拖尾”。
3)对比不同初始Eh土壤中单一重金属Cd、Zn、Cu的BTCs发现,氧化性土壤中Cd、Zn、Cu运移较快,表现为出流较早,峰值较高；而还原性土壤能明显促进Cd的迁移,抑制Cu的迁移,对Zn迁移的影响并不明显。出流液pH的变化是先下降后上升最后趋于平缓,Eh的变化则是先上升后下降最后趋于平缓。
4)在两种重金属离子Cd、Zn的共存实验中,重金属出流的拐点比单一离子时出现的提前,峰值也要高,这说明共存条件下,Cd、Zn共同利用吸附点位而使吸附受到彼此牵制。Cd、Zn共存迁移时,出流液pH比单一重金属离子时的相对要低,Eh相对要高,共存迁移时Ec低于单一重金属离子存在时的Ec,可能主要是受土壤颗粒表面吸附的阳离子的导电性的影响。
5)在两种重金属离子Cd/Cu、Zn/Cu的共存实验中,重金属Cd/Zn的穿透曲线出流拐点比Cu的穿透曲线要提前,峰值也要高,这主要是因为共存时,重金属的不同迁移规律可能与重金属水解能力强弱有关。不同初始Eh的土壤中,与单一重金属离子存在时相比,共存迁移出流液pH都最低,Eh最高,Ec最低。当三种重金属共存迁移时,出流液峰值顺序为：Zn2+>Cd2+> Cu2+,这主要是受不同重金属离子的离子半径、原子量、水解常数和软度系数等性质的影响。
6)利用平衡模型对Br的BTCs进行拟合,得到r2>0.98, MSE<0.006,表明Br-的BTCs能被平衡模型较好的拟合,拟合得到的参数可用于Cd、Zn、Cu运移的数值模拟。将静态吸附的数据,用Langmuir、Freundlich方程求得Rd值用于重金属拟合过程,能够更好地了解重金属在不同初始Eh土壤中的吸附特性。
7)由单点吸附模型对不同初始Eh土壤中重金属Cd、Zn、Cu的迁移行为进行描述可以看出,BTCs拟合的r2>0.814, MSE<0.028,这说明应用单点吸附模型能较好地描述重金属的迁移行为,单点吸附模型拟合的β值普遍较小,质量传递系数ω远小于100。本文还应用单点吸附模型预测了不同初始Eh土壤中,不同深度处出流液中重金属浓度的动态变化,随着深度由5cm增加到15cm,它们的相对浓度对孔隙体积的响应均表现滞后。
Soil chemical environment is one of the important environmental factors in a human life, which affects plant growth and development, to a large extent restricts the quality of food. However, Soil chemical environment is vulnerable to heavy metal contamination of materials. The heavy metals which are introduced into the soils either accumulate in the surface layer or transport into the groundwater. Redox reaction is a basic soil chemical and biochemical processes, which changs the valence state of ions in soil affected by the presence of inorganic and organic forms, migration and transformation. Redox potential plays an important role on various chemical, biological processes of the soil. Therefore the study of transport processes is of utmost importance for the evaluation of environmental risks.
First of all, the present study evaluates the adsorption and competitive adsorption of three heavy metals (Cd, Zn, Cu) in five different initial redox potential of soils by means of sorption isotherms, evaluates the capacity of these soils to sorb these metals. And then, we are to evaluate the transport and competitive transport of the metals (Cd, Zn, Cu) in these soils based on miscible displacement experiments and HYDRUS-1D package is used to determine model parameters and predict the outflow dynamics. The conclusions have been drawn as followed:
In the static adsorption isotherm experiment, five different initial redox potential of soils have significant differences of adsorption capacity of a single heavy metal, reduced soil> brown> oxidized soil. The adsorption amounts of heavy metals in soils are increased with its increasing equilibrium concentration. The adsorption amounts of two ions in the competitive experiment are less than that in single system. Coexistence of three heavy metal ions, the sequence of the competitiveness of three heavy metals is Cu2+>Cd2+>Zn2+. With its increasing equilibrium concentration, pH is decreased, Eh is increased and Ec is increased. In this paper, the Freundlich equation is more accurately than the Langmuir equqtion to describe adsorption behavior of three heavy metals.
Compared with the BTCs of Br", the five different initial redox potential of soils can obviously influence the shape and peak values of the BTCs of heavy metals. The BTCs of heavy metals from the transport experiment are exceedingly asymmetric.
In the five different initial redox potential of soils, compared with the BTCs of heavy metals, it was found that the initial redox potential were positively correlated with the transport of heavy metals. The change of the leachate pH is degressive, then leveling off. The change of the leachate Eh is increased, then leveling off.
In the competitive experiment of Cd and Zn, the resident concentration of heavy metals was higher than that in the single system. The total adsorption of heavy metals (the amount of the Cd and Zn competitive adsorption) than a single condition in the adsorption is significantly lower. The change of the leachate pH in the competitive experiment is lower than single ion and the Eh is the higher, the Ec is the lower.
Compared with the competitive experiment of Cd and Cu, Zn and Cu, in the single-ion experiments, it was found that the flow time of copper is higher than that of cadmium/zinc, the peak value of copper is higher than that of cadmium/zinc in the oxidized soil, the peak value of the reduced soil is lower than the oxidized soil. In the competitive experiment, the resident concentration of heavy metals was higher than that in the single system. The change of the leachate pH in the competitive experiment is lower than single ion and the Eh is the higher, the Ec is the lower.In the competitive experiment, the sequence of the capacity of the three heavy metals adsorption by the soils was Zn>Cd>Cu. It can be explained by the hydrolysis capacity, atomic weight, the hydrolysis constant and coefficient of soft.
The BTCs of Br- can all be fitted by One-site sorption model with high goodness of fit(r2>0.98, MSE<0.006). When we use the retardation factor to fit the BTCs, we find the retardation factors from Freundlich are suitable in most cases, which can understand the initial redox potential of heavy metals in soils of different adsorption characteristics.
The BTCs of heavy metals in soil column can all be fitted by One-site sorption model with high goodness of fit (r2>0.814, MSE<0.028). Through these model parameters acquired by the One-site sorption model, we can predict the BTCs of heavy metals at different depth of soil columns. As the depth of soil column increased from 5cm to 15cm, the hysterestic effect of response of relative concentration of heavy metals to the pore volumes will be more and more obvious.
本文以较为常见的镉、锌、铜三种重金属作为研究对象,以五种不同初始氧化还原电位(Eh)的土壤为介质,首先研究了静态情况下,三种重金属的吸附、竞争吸附特性；接着重点研究了三种重金属在五种不同初始Eh土壤中的迁移规律,并进一步探讨了多种重金属共存时,竞争吸附作用对其迁移规律和作用机理的影响,并应用美国盐土实验室研制的HYDRUS-1D软件,模拟了重金属在土壤中的穿透曲线,获得了拟合参数；最后运用这些参数对土壤不同埋深条件下重金属的迁移行为进行预测。得出以下结论：
1)在静态等温吸附实验中,五种不同初始Eh土壤对单一重金属离子的吸附量存在很大差别,还原性土壤>原棕壤>氧化性土壤；随着平衡液中重金属浓度的增加,土壤对重金属的吸附量呈增大趋势。当两种重金属共存时,土壤对单一重金属的吸附量要大于两种重金属共存时的吸附量；三种重金属离子共存时,重金属离子的竞争吸附能力大小顺序为：Cu2+>Cd2+>Zn2+。另外,随着平衡液中重金属浓度的增大,平衡液的pH呈下降趋势,Eh呈现上升趋势且均高于土壤初始Eh,平衡液的电导率(Ec)呈上升趋势,且氧化性土壤的Ec大于还原性土壤的Ec。用Langmuir方程和Freundlich方程对数据进行拟合,确定性系数R2都在0.948以上,总体拟合效果较好,Freundlich方程的拟合效果更佳。
2)Br-在棕壤中迁移的穿透曲线(BTCs)具有较好的对称性,说明土壤的物理非平衡影响较小。与Br-的BTCs相比,不同初始Eh土壤对三种重金属BTCs的形状和峰值等都有影响,所有能检测出重金属的BTCs均呈现出不同程度的非对称性,解吸部分有较长的“拖尾”。
3)对比不同初始Eh土壤中单一重金属Cd、Zn、Cu的BTCs发现,氧化性土壤中Cd、Zn、Cu运移较快,表现为出流较早,峰值较高；而还原性土壤能明显促进Cd的迁移,抑制Cu的迁移,对Zn迁移的影响并不明显。出流液pH的变化是先下降后上升最后趋于平缓,Eh的变化则是先上升后下降最后趋于平缓。
4)在两种重金属离子Cd、Zn的共存实验中,重金属出流的拐点比单一离子时出现的提前,峰值也要高,这说明共存条件下,Cd、Zn共同利用吸附点位而使吸附受到彼此牵制。Cd、Zn共存迁移时,出流液pH比单一重金属离子时的相对要低,Eh相对要高,共存迁移时Ec低于单一重金属离子存在时的Ec,可能主要是受土壤颗粒表面吸附的阳离子的导电性的影响。
5)在两种重金属离子Cd/Cu、Zn/Cu的共存实验中,重金属Cd/Zn的穿透曲线出流拐点比Cu的穿透曲线要提前,峰值也要高,这主要是因为共存时,重金属的不同迁移规律可能与重金属水解能力强弱有关。不同初始Eh的土壤中,与单一重金属离子存在时相比,共存迁移出流液pH都最低,Eh最高,Ec最低。当三种重金属共存迁移时,出流液峰值顺序为：Zn2+>Cd2+> Cu2+,这主要是受不同重金属离子的离子半径、原子量、水解常数和软度系数等性质的影响。
6)利用平衡模型对Br的BTCs进行拟合,得到r2>0.98, MSE<0.006,表明Br-的BTCs能被平衡模型较好的拟合,拟合得到的参数可用于Cd、Zn、Cu运移的数值模拟。将静态吸附的数据,用Langmuir、Freundlich方程求得Rd值用于重金属拟合过程,能够更好地了解重金属在不同初始Eh土壤中的吸附特性。
7)由单点吸附模型对不同初始Eh土壤中重金属Cd、Zn、Cu的迁移行为进行描述可以看出,BTCs拟合的r2>0.814, MSE<0.028,这说明应用单点吸附模型能较好地描述重金属的迁移行为,单点吸附模型拟合的β值普遍较小,质量传递系数ω远小于100。本文还应用单点吸附模型预测了不同初始Eh土壤中,不同深度处出流液中重金属浓度的动态变化,随着深度由5cm增加到15cm,它们的相对浓度对孔隙体积的响应均表现滞后。
Soil chemical environment is one of the important environmental factors in a human life, which affects plant growth and development, to a large extent restricts the quality of food. However, Soil chemical environment is vulnerable to heavy metal contamination of materials. The heavy metals which are introduced into the soils either accumulate in the surface layer or transport into the groundwater. Redox reaction is a basic soil chemical and biochemical processes, which changs the valence state of ions in soil affected by the presence of inorganic and organic forms, migration and transformation. Redox potential plays an important role on various chemical, biological processes of the soil. Therefore the study of transport processes is of utmost importance for the evaluation of environmental risks.
First of all, the present study evaluates the adsorption and competitive adsorption of three heavy metals (Cd, Zn, Cu) in five different initial redox potential of soils by means of sorption isotherms, evaluates the capacity of these soils to sorb these metals. And then, we are to evaluate the transport and competitive transport of the metals (Cd, Zn, Cu) in these soils based on miscible displacement experiments and HYDRUS-1D package is used to determine model parameters and predict the outflow dynamics. The conclusions have been drawn as followed:
In the static adsorption isotherm experiment, five different initial redox potential of soils have significant differences of adsorption capacity of a single heavy metal, reduced soil> brown> oxidized soil. The adsorption amounts of heavy metals in soils are increased with its increasing equilibrium concentration. The adsorption amounts of two ions in the competitive experiment are less than that in single system. Coexistence of three heavy metal ions, the sequence of the competitiveness of three heavy metals is Cu2+>Cd2+>Zn2+. With its increasing equilibrium concentration, pH is decreased, Eh is increased and Ec is increased. In this paper, the Freundlich equation is more accurately than the Langmuir equqtion to describe adsorption behavior of three heavy metals.
Compared with the BTCs of Br", the five different initial redox potential of soils can obviously influence the shape and peak values of the BTCs of heavy metals. The BTCs of heavy metals from the transport experiment are exceedingly asymmetric.
In the five different initial redox potential of soils, compared with the BTCs of heavy metals, it was found that the initial redox potential were positively correlated with the transport of heavy metals. The change of the leachate pH is degressive, then leveling off. The change of the leachate Eh is increased, then leveling off.
In the competitive experiment of Cd and Zn, the resident concentration of heavy metals was higher than that in the single system. The total adsorption of heavy metals (the amount of the Cd and Zn competitive adsorption) than a single condition in the adsorption is significantly lower. The change of the leachate pH in the competitive experiment is lower than single ion and the Eh is the higher, the Ec is the lower.
Compared with the competitive experiment of Cd and Cu, Zn and Cu, in the single-ion experiments, it was found that the flow time of copper is higher than that of cadmium/zinc, the peak value of copper is higher than that of cadmium/zinc in the oxidized soil, the peak value of the reduced soil is lower than the oxidized soil. In the competitive experiment, the resident concentration of heavy metals was higher than that in the single system. The change of the leachate pH in the competitive experiment is lower than single ion and the Eh is the higher, the Ec is the lower.In the competitive experiment, the sequence of the capacity of the three heavy metals adsorption by the soils was Zn>Cd>Cu. It can be explained by the hydrolysis capacity, atomic weight, the hydrolysis constant and coefficient of soft.
The BTCs of Br- can all be fitted by One-site sorption model with high goodness of fit(r2>0.98, MSE<0.006). When we use the retardation factor to fit the BTCs, we find the retardation factors from Freundlich are suitable in most cases, which can understand the initial redox potential of heavy metals in soils of different adsorption characteristics.
The BTCs of heavy metals in soil column can all be fitted by One-site sorption model with high goodness of fit (r2>0.814, MSE<0.028). Through these model parameters acquired by the One-site sorption model, we can predict the BTCs of heavy metals at different depth of soil columns. As the depth of soil column increased from 5cm to 15cm, the hysterestic effect of response of relative concentration of heavy metals to the pore volumes will be more and more obvious.
引文
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