多孔介质中重金属反应性运移的数值模拟研究
摘要
为充分研究不同理化因素对重金属在土壤中运移的影响,降低不同因素之间的相互干扰,本文选取低反应性多孔介质石英砂为介质,在条件可控的情况下进行多种重金属反应性运移实验和数值模拟研究,进而为分析重金属污染土壤中多组分反应性运移行为及重金属污染修复提供科学依据。
本研究分别开展了Cu~(2+)、pb~(2+)、Zn~(2+)和Cd~(2+)单组分和多组分溶液的室内石英砂柱出流实验,并对每种重金属进行了改变pH值、改变脉冲溶液流速和改变离子强度的出流实验。
采用梯度正则化方法对一维溶质运移方程中源(汇)项的敏感性、实验数据误差影响和弥散系数敏感性进行了分析。
实验数据误差对数值模拟影响的分析表明,误差小于5%时数值解和精确解之间的误差比较小,不同正则化参数对数值解影响比较小,但对迭代收敛速度影响比较大;误差大于10%时,不同正则化参数对数值解影响比较大。数值模拟中最终实测数据的获得需要在石英砂柱的不同切面处采集溶液,难以实现,本文采用出流端拟合曲线得到的数据,这可能也是数值模拟过程中拟合精度有所降低的原因。
本研究利用CXTFIT软件(只考虑对流弥散作用)进行常规溶质运移的模拟,利用PHREEQC软件(考虑离子交换和吸附作用)进行耦合化学反应的溶质运移模拟,实验和模拟结果表明:
随孔隙水流速增加,重金属离子出流、到达峰值结束的时间逐渐提前;随着pH值从7减小到4,重金属离子峰值逐渐增大,pH越低,重金属的出流提前,峰值变高;增加离子强度,重金属离子的穿透曲线具有相似特征,均为随着溶液背景离子强度的增大,出流峰值增大;重金属离子混合溶液中离子强度大于单一组分溶液离子强度,出流液中出流峰值与单一组分溶液出流峰值相比也有明显增加,这与增加溶液背景离子强度的结果一致,说明增加离子强度可以加快重金属在多孔介质中的运移,降低石英砂对重金属离子的吸附。
对于单一重金属离子运移的模拟,CXTFIT软件和PHREEQC软件拟合精确度均较高,决定系数及MSE相差不大,这主要是单一重金属离子在多孔介质中的吸附、离子交换等反应相对简单,而对于多组分重金属离子在多孔介质中运移的模拟,PHREEQC软件模拟结果要优于CXTFIT软件的模拟结果,这与PHREEQC软件模拟过程中考虑了吸附、离子交换等反应有关。
对于不同理化条件下重金属离子的运移,从拟合的决定系数平均值来看,Cu~(2+)、Zn~(2+)和Cd~(2+)的拟合度要优于Pb~(2+)的拟合度,这主要是因为Pb~(2+)的吸附强度较高,而且Pb~(2+)在石英砂柱中发生的反应较Cu~(2+)、Zn~(2+)、Cd~(2+)复杂,模拟难度加大,模拟精度有所降低,对比吸附解吸两个阶段的模拟精度,吸附阶段模拟精度较高,在解吸阶段精度下降很大。
石英砂柱出流液中随着重金属组分的增加,出流液峰值随之增加,并且出现输出浓度大于输入浓度(C/C_0大于1)的情况,主要原因是受层析原理的影响,对Cd~(2+)的影响要大于其它三种重金属,Cu~(2+)、Pb~(2+)、Zn~(2+)、Cd~(2+)多组分溶液中Cd~(2+)出流峰值C/C_0最大值为1.526,这说明多组分在多孔介质中运移的过程中,层析现象对Cd~(2+)的影响要大于其它三种重金属,这主要是受重金属水解能力强弱的主导,水解常数pK:Pb~(2+)(7.8)＞Cu~(2+)(8.0)＞Zn~(2+)(9.0)＞Cd~(2+)(10.1)。多组分重金属出流输出浓度大于输入浓度(C/C_0大于1)情况对于数值模拟的影响也较为明显,模拟精确度有所降低。
为预测极端情况下多组分重金属离子在高盐或高pH值溶液中的运移规律,利用前面已经调试的PHREEQC软件对高盐(0.25mol/l)和高pH值(pH=7.5)进行模拟,模拟情况与已知实验结果较为吻合。
本文顾及到了组分之间的相互作用,并在水动力弥散过程中耦合了吸附、离子交换等化学反应,能够较好的反映实际情况,为重金属污染多孔介质的评估、修复提供科学依据。
In order to fully study the effect of different physical and chemical factors on the transport of heavy metals in soil,this dissertation studies on four heavy metals which were conducted in small columns full with low-reactive quartz sand under control conditions to obtain precise data and exclude the effect of unknown aspects.
On controllable condition in lab,each column was added single or multicomponents of heavy metal ions and the influences of different pH,flow velocity and ionic strength on these ions transport were studied.
The source and sinks term,sensitivity,data error and dispersion coefficient sensitivity for one-dimensional advection-dispersion equation(CDE)were analyzed through gradient-regularization algorithm.
The analysis indicated that if the data error of experiment was less than 5%the numerical solution accorded with the true solution very well,if the data error was more than 10%,it would affect the simulation.Also,the data of BTCs affected the precision of the simulation.
To each experiment,traditional solute transport without chemical reaction was simulated by computer program CXTFIT and coupled chemical reaction solute transport was simulated by the hydrologic geochemical software PHREEQC.The results revealed:
Breakthrough time and arrival of peak concentration became earler with the flow velocity increased from 0.05 m/h to 0.3 m/h.The capacity of heavy metals adsorbed on quartz sand decreased in low pH conditions with high peak concentration.There was also earlier breakthrough with the similar BTCs with the ions strength increased.
It was well accorded between CXTFIT and PHREEQC in simulation of single heavy metal because the simplification of chemical reaction.The simulation coupled adsorption (with PHREEQC)was better than non-coupled one(with CXTFIT)and it could describe experimental results successfully because the PHREEQC software took into account the reactions of adsorption and ion exchanging.
The simulation of the heavy metal Cu~(2+),Zn~(2+),Cd~(2+) was better than the simulation of the heavy metal Pb~(2+)because of the difference of the adsorption.
The peak concentration significantly increased in multicomponents condition compared with single component condition,which also indicated that the increased ions strength could facilitate heavy metals transport and decrease retention in columns.It had a peak concentration that exceeded the input concentration(C/C_0＞1.0),especially in Cd solution.It indicated that the hydrolysis constant was the important effactor for the chromatographic or snow-plow effect.The chromatographic effect also affected the simulation for the experimental data.
The simulation in the high salt(0.25mol/l)and high pH(pH=7.5)condition accorded well with the experimental data.
The simulation of solute transport was coupled with chemical reactive such as adsorption and ions exchange,which could reflect the real conditions and provid references for the evaluation and remediation of contaminated soils by heavy metals.
本研究分别开展了Cu~(2+)、pb~(2+)、Zn~(2+)和Cd~(2+)单组分和多组分溶液的室内石英砂柱出流实验,并对每种重金属进行了改变pH值、改变脉冲溶液流速和改变离子强度的出流实验。
采用梯度正则化方法对一维溶质运移方程中源(汇)项的敏感性、实验数据误差影响和弥散系数敏感性进行了分析。
实验数据误差对数值模拟影响的分析表明,误差小于5%时数值解和精确解之间的误差比较小,不同正则化参数对数值解影响比较小,但对迭代收敛速度影响比较大;误差大于10%时,不同正则化参数对数值解影响比较大。数值模拟中最终实测数据的获得需要在石英砂柱的不同切面处采集溶液,难以实现,本文采用出流端拟合曲线得到的数据,这可能也是数值模拟过程中拟合精度有所降低的原因。
本研究利用CXTFIT软件(只考虑对流弥散作用)进行常规溶质运移的模拟,利用PHREEQC软件(考虑离子交换和吸附作用)进行耦合化学反应的溶质运移模拟,实验和模拟结果表明:
随孔隙水流速增加,重金属离子出流、到达峰值结束的时间逐渐提前;随着pH值从7减小到4,重金属离子峰值逐渐增大,pH越低,重金属的出流提前,峰值变高;增加离子强度,重金属离子的穿透曲线具有相似特征,均为随着溶液背景离子强度的增大,出流峰值增大;重金属离子混合溶液中离子强度大于单一组分溶液离子强度,出流液中出流峰值与单一组分溶液出流峰值相比也有明显增加,这与增加溶液背景离子强度的结果一致,说明增加离子强度可以加快重金属在多孔介质中的运移,降低石英砂对重金属离子的吸附。
对于单一重金属离子运移的模拟,CXTFIT软件和PHREEQC软件拟合精确度均较高,决定系数及MSE相差不大,这主要是单一重金属离子在多孔介质中的吸附、离子交换等反应相对简单,而对于多组分重金属离子在多孔介质中运移的模拟,PHREEQC软件模拟结果要优于CXTFIT软件的模拟结果,这与PHREEQC软件模拟过程中考虑了吸附、离子交换等反应有关。
对于不同理化条件下重金属离子的运移,从拟合的决定系数平均值来看,Cu~(2+)、Zn~(2+)和Cd~(2+)的拟合度要优于Pb~(2+)的拟合度,这主要是因为Pb~(2+)的吸附强度较高,而且Pb~(2+)在石英砂柱中发生的反应较Cu~(2+)、Zn~(2+)、Cd~(2+)复杂,模拟难度加大,模拟精度有所降低,对比吸附解吸两个阶段的模拟精度,吸附阶段模拟精度较高,在解吸阶段精度下降很大。
石英砂柱出流液中随着重金属组分的增加,出流液峰值随之增加,并且出现输出浓度大于输入浓度(C/C_0大于1)的情况,主要原因是受层析原理的影响,对Cd~(2+)的影响要大于其它三种重金属,Cu~(2+)、Pb~(2+)、Zn~(2+)、Cd~(2+)多组分溶液中Cd~(2+)出流峰值C/C_0最大值为1.526,这说明多组分在多孔介质中运移的过程中,层析现象对Cd~(2+)的影响要大于其它三种重金属,这主要是受重金属水解能力强弱的主导,水解常数pK:Pb~(2+)(7.8)＞Cu~(2+)(8.0)＞Zn~(2+)(9.0)＞Cd~(2+)(10.1)。多组分重金属出流输出浓度大于输入浓度(C/C_0大于1)情况对于数值模拟的影响也较为明显,模拟精确度有所降低。
为预测极端情况下多组分重金属离子在高盐或高pH值溶液中的运移规律,利用前面已经调试的PHREEQC软件对高盐(0.25mol/l)和高pH值(pH=7.5)进行模拟,模拟情况与已知实验结果较为吻合。
本文顾及到了组分之间的相互作用,并在水动力弥散过程中耦合了吸附、离子交换等化学反应,能够较好的反映实际情况,为重金属污染多孔介质的评估、修复提供科学依据。
In order to fully study the effect of different physical and chemical factors on the transport of heavy metals in soil,this dissertation studies on four heavy metals which were conducted in small columns full with low-reactive quartz sand under control conditions to obtain precise data and exclude the effect of unknown aspects.
On controllable condition in lab,each column was added single or multicomponents of heavy metal ions and the influences of different pH,flow velocity and ionic strength on these ions transport were studied.
The source and sinks term,sensitivity,data error and dispersion coefficient sensitivity for one-dimensional advection-dispersion equation(CDE)were analyzed through gradient-regularization algorithm.
The analysis indicated that if the data error of experiment was less than 5%the numerical solution accorded with the true solution very well,if the data error was more than 10%,it would affect the simulation.Also,the data of BTCs affected the precision of the simulation.
To each experiment,traditional solute transport without chemical reaction was simulated by computer program CXTFIT and coupled chemical reaction solute transport was simulated by the hydrologic geochemical software PHREEQC.The results revealed:
Breakthrough time and arrival of peak concentration became earler with the flow velocity increased from 0.05 m/h to 0.3 m/h.The capacity of heavy metals adsorbed on quartz sand decreased in low pH conditions with high peak concentration.There was also earlier breakthrough with the similar BTCs with the ions strength increased.
It was well accorded between CXTFIT and PHREEQC in simulation of single heavy metal because the simplification of chemical reaction.The simulation coupled adsorption (with PHREEQC)was better than non-coupled one(with CXTFIT)and it could describe experimental results successfully because the PHREEQC software took into account the reactions of adsorption and ion exchanging.
The simulation of the heavy metal Cu~(2+),Zn~(2+),Cd~(2+) was better than the simulation of the heavy metal Pb~(2+)because of the difference of the adsorption.
The peak concentration significantly increased in multicomponents condition compared with single component condition,which also indicated that the increased ions strength could facilitate heavy metals transport and decrease retention in columns.It had a peak concentration that exceeded the input concentration(C/C_0＞1.0),especially in Cd solution.It indicated that the hydrolysis constant was the important effactor for the chromatographic or snow-plow effect.The chromatographic effect also affected the simulation for the experimental data.
The simulation in the high salt(0.25mol/l)and high pH(pH=7.5)condition accorded well with the experimental data.
The simulation of solute transport was coupled with chemical reactive such as adsorption and ions exchange,which could reflect the real conditions and provid references for the evaluation and remediation of contaminated soils by heavy metals.
引文
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