地下水有机物和重金属迁移与污染修复的数值模拟研究
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摘要
地下水污染带来的环境健康风险和生态安全已受到人们的极大关注。2011年10月10日国务院正式批复了《全国地下水污染防治规划(2011-2020)》，这是我国地下水污染防治的第一部纲领性文件，标志着地下水这一战略资源的污染防治工作已经纳入国家层面的决策。纵观当前地下水污染状况，非水相重质液体(Dense Non-Aqueous Phase Liquids,DNAPLs)、非水相轻质液体(Light Non-Aqueous Phase Liquids, LNAPLs)和重金属类污染物已经成为目前地下水污染控制的重中之重，于是选取了四氯乙烯、苯、六价铬作为本文的研究对象。此外，随着计算机技术的迅速发展，数值模拟技术已经成了研究地下水污染物迁移与修复过程的重要工具。因此，用数值模拟研究这三种污染物在地下水中的迁移规律与修复方案的制定，具有非常重要的科学研究和实际应用价值。
基于本课题组多年来地下水污染修复试验之上，以地下水数值模拟软件应该坚持自主开发与引进相结合为原则，利用美国地质调查局(USGS)开发的MODFLOW-2005和美国阿拉巴马大学(UA)Prof. Chunmiao Zheng开发的MT3DMS源程序代码，开发了能实现多组分一级母-子连锁反应，多元莫诺动力学反应，重金属吸附和化学淤堵作用的计算模拟程序，主要研究成果如下。
针对以铁粉与微生物群落组合(FeMB)为反应材料的多级PRB(Permeable Reactive Barrier)修复四氯乙烯(PCE)污染含水层的过程，建立了多组分一级母-子连锁反应模型，开发相应程序。结果表明，(1)质量转化系数对PCE由非水相向水相的转化过程非常重要，直接影响到非水相PCE污染源的存在时间和水相中PCE的浓度峰值；(2)FeMB作PRB反应材料的生物化学降解作用在PCE的去除过程中起主导性作用；(3)2级PRB的修复效果与1级相比，浓度峰值降低了37%；3级与2级相比，浓度峰值又降低了36%，因此在污染修复过程中出现中间产物时，多级PRB是一种可行的修复技术；(4)在地下水修复过程中，反应材料降解性能衰减和渗透性的减小直接影响最终的修复效果，应引起足够的重视。
针对缓慢注氧(Slow-release Oxygen Source, SOS)或PRB缓慢释氧(Oxygen-Releasing Compounds, ORC)技术修复苯污染含水层的过程，建立苯、溶解氧和微生物的多元莫诺动力学反应模型，开发相应程序。结果表明，(1)注氧井离污染源越近有助于达到更好的修复效果，充足的溶解氧能够加速微生物的生长过程，使更多的苯在微生物生长过程中被消耗掉；(2)汽油的饱和度直接决定着其在非饱和带的垂向迁移速度，大部分汽油都被非饱和带所截留，给土壤和近地表生态环境带来了潜在的危害；(3)PRB释氧速率15mg/L的方案使苯的浓度峰值在处理前后下降了80%，饱和带中苯污染羽主要集中于近地下水面附近，PRB设计过程中应予以充分地考虑；(4)缓慢注氧(SOS)技术和PRB缓慢释氧(ORC)技术是很好的补充地下水中溶解氧的方式。
针对六价铬(Cr~(6+))柱实验，采用遗传算法开发了吸附参数反演模型，然后以改性壳聚糖(PEG-CTS#5)为吸附剂设计了PRB的最佳尺寸结构。结果表明，(1)以MODFLOW/MT3DMS为工具，根据六价铬浓度0.1mg/L的污染羽范围设计PRB尺寸的方法是可行的；(2)PEG-CTS#5应该是一种潜在吸附六价铬的材料，但该材料遇水后膨胀进而影响反应区的渗透性，应引起足够的重视；(3)弥散度在横向和垂向上的增大将使PRB厚度减小，长度和深度增加，介质弥散度的异质性对PRB的设计非常关键。
针对地下水修复过程中的化学淤堵现象，建立了由二价铁离子(Fe~(2+))引起的辐射集水井化学淤堵模型，开发相应程序。结果表明，(1)建立的辐射集水井出水量模型是可行的，就辐射井的水平集水管而言，末端的出水量贡献大于靠近井中心处的出水量；(2)辐射井竖井发生化学淤堵，45天后的出水量下降约10%～15%，含水层水位上升，给相关工程带来一定的安全隐患。
Groundwater contamination has led to environmental health risk andecological safety. This problem has been more and more attention togovernment and environmental scientists. In October10,2011, the Chinesegovernment passed the “National Groundwater Contamination Prevention andRemediation Plan (2011-2020)”. The plan is the first programmatic documentof groundwater contamination prevention and remediation in China. Itindicates that groundwater contamination prevention and remediation havebeen included in decision-making at national level. As far as the current stateof groundwater contamination is concerned, there are the following threetypes of contamination: Dense non-aqueous phase liquids (DNAPLs), Lightnon-aqueous phase liquids (LNAPLs) and heavy metals. They have becomethe top priority of groundwater contamination prevention and remediation.Thereby, perchloroethylene (PCE), benzene and hexavalent chromium (Cr~(6+))are chosed as target contaminants in the paper. In addition, with the rapiddevelopment of computer technology, numerical simulation has become animportant tool to study transport and remediation process of contaminant ingroundwater. Therefore, it is a very meaningful work about researchingtransport and remediation law of the three pollutants by numerical simulationtechnique.
Based on some groundwater remediation tests performed by our researchgroup in the past few years, we adhere to combination of self-developmentand introduction for groundwater numerical simulation software, and developprogram codes that can perform the following functions: multispecies mother-daughter kinetic reactions, Monod kinetics reactions, adsorption andchemical clogging of heavy metals. The program codes are on the basis ofMODFLOW-2005developed by USGS and MT3DMS developed by Prof.Chunmiao Zheng in University of Alabama. The main results can be writtenas follows.
For PCE-contaminated aquifer repaired by multi-PRB using iron andmicrobial community (FeMB) as reactive media, it built the multispeciesmother-daughter kinetic reactions model and developed its program codes.The results showed that (1) the bulk mass transfer coefficient was veryimportant for PCE transfering from non-aqueous phase to aqueous phase, andaffected the dissolution time and concentration peak,(2) thebiological/chemical reaction of PRB using FeMB as reactive media wasdominant in remediation process,(3) the concentration peak of two-stagePRB had a37%decrease comparing with that of one-stage, the value ofthree-stage had also a36%decrease comparing with that of two-stage,therefore multi-PRB could be a preferred option for intermediate products inremediation process,(4) the losses of reaction rate and hydraulic conductivitycan cause a decline of remediation effect.
For benzene-contaminzted aquifer repaired by slow-release oxygensource (SOS) technique and PRB with oxygen-releasing compounds (ORC),it built the Monod kinetics reactions model including benzene, DO andmicrobial species, and developed its program codes. The results showed that(1) placing the release oxygen well closer to source was more efficient,enough DO maybe accelerate the growth of microbial species which couldconsume more benzene,(2) the vertical velocity of gasoline in unsaturatedzone was dominates by its saturation, the most of gasoline was trapped byunsaturated zone after gasoline spills, it would cause potential risk of soilecological environment,(3) the scenario of oxygen-releasing rate15mg/Lcould have a80%decrease of benzene concentration in treated groundwater,the contaminant plume of benzene in saturated zone was near groundwatertable, it should be considered for PRB design,(4) the SOS and PRB with ORC were potential methods that can provide oxygen for groundwater.
For a column test of hexavalent chromium (Cr~(6+)), it developed aparameter estimation model for adsorption using genetic algorthms, thendesigned the PRB’s optimal size using modified chitosan (PEG-CTS#5) asreactive media. The results showed that (1) using MODFLOW/MT3DMS astool, the design method was appropriate on the based of the contaminantplume of0.1mg/L for Cr~(6+),(2) PEG-CTS#5may be a potential adsorptionmedium to restore Cr~(6+)-contaminated groundwater, but it would bulge ingroundwater and clog the flow,(3) the increase of horizontal and verticaltransverse dispersivity would decrease the PRB’s width and increase thelength and height, the heterogeneity was very important for PRB’s design.
For chemical clogging in groundwater remediation, it built a modelconsidering the chemical clogging around radial collector well, and developedits program codes. The results showed that (1) the model computing the waterdischarge of radial collector well was reasonable, the water discharge inbottom of horizontal screen lateral was bigger than that near the center of well,(2) the water discharge of radial collector well after45days declined by10-15%due to the chemical clogging, the groundwater table would raise andfinally influence engineering safety.
基于本课题组多年来地下水污染修复试验之上，以地下水数值模拟软件应该坚持自主开发与引进相结合为原则，利用美国地质调查局(USGS)开发的MODFLOW-2005和美国阿拉巴马大学(UA)Prof. Chunmiao Zheng开发的MT3DMS源程序代码，开发了能实现多组分一级母-子连锁反应，多元莫诺动力学反应，重金属吸附和化学淤堵作用的计算模拟程序，主要研究成果如下。
针对以铁粉与微生物群落组合(FeMB)为反应材料的多级PRB(Permeable Reactive Barrier)修复四氯乙烯(PCE)污染含水层的过程，建立了多组分一级母-子连锁反应模型，开发相应程序。结果表明，(1)质量转化系数对PCE由非水相向水相的转化过程非常重要，直接影响到非水相PCE污染源的存在时间和水相中PCE的浓度峰值；(2)FeMB作PRB反应材料的生物化学降解作用在PCE的去除过程中起主导性作用；(3)2级PRB的修复效果与1级相比，浓度峰值降低了37%；3级与2级相比，浓度峰值又降低了36%，因此在污染修复过程中出现中间产物时，多级PRB是一种可行的修复技术；(4)在地下水修复过程中，反应材料降解性能衰减和渗透性的减小直接影响最终的修复效果，应引起足够的重视。
针对缓慢注氧(Slow-release Oxygen Source, SOS)或PRB缓慢释氧(Oxygen-Releasing Compounds, ORC)技术修复苯污染含水层的过程，建立苯、溶解氧和微生物的多元莫诺动力学反应模型，开发相应程序。结果表明，(1)注氧井离污染源越近有助于达到更好的修复效果，充足的溶解氧能够加速微生物的生长过程，使更多的苯在微生物生长过程中被消耗掉；(2)汽油的饱和度直接决定着其在非饱和带的垂向迁移速度，大部分汽油都被非饱和带所截留，给土壤和近地表生态环境带来了潜在的危害；(3)PRB释氧速率15mg/L的方案使苯的浓度峰值在处理前后下降了80%，饱和带中苯污染羽主要集中于近地下水面附近，PRB设计过程中应予以充分地考虑；(4)缓慢注氧(SOS)技术和PRB缓慢释氧(ORC)技术是很好的补充地下水中溶解氧的方式。
针对六价铬(Cr~(6+))柱实验，采用遗传算法开发了吸附参数反演模型，然后以改性壳聚糖(PEG-CTS#5)为吸附剂设计了PRB的最佳尺寸结构。结果表明，(1)以MODFLOW/MT3DMS为工具，根据六价铬浓度0.1mg/L的污染羽范围设计PRB尺寸的方法是可行的；(2)PEG-CTS#5应该是一种潜在吸附六价铬的材料，但该材料遇水后膨胀进而影响反应区的渗透性，应引起足够的重视；(3)弥散度在横向和垂向上的增大将使PRB厚度减小，长度和深度增加，介质弥散度的异质性对PRB的设计非常关键。
针对地下水修复过程中的化学淤堵现象，建立了由二价铁离子(Fe~(2+))引起的辐射集水井化学淤堵模型，开发相应程序。结果表明，(1)建立的辐射集水井出水量模型是可行的，就辐射井的水平集水管而言，末端的出水量贡献大于靠近井中心处的出水量；(2)辐射井竖井发生化学淤堵，45天后的出水量下降约10%～15%，含水层水位上升，给相关工程带来一定的安全隐患。
Groundwater contamination has led to environmental health risk andecological safety. This problem has been more and more attention togovernment and environmental scientists. In October10,2011, the Chinesegovernment passed the “National Groundwater Contamination Prevention andRemediation Plan (2011-2020)”. The plan is the first programmatic documentof groundwater contamination prevention and remediation in China. Itindicates that groundwater contamination prevention and remediation havebeen included in decision-making at national level. As far as the current stateof groundwater contamination is concerned, there are the following threetypes of contamination: Dense non-aqueous phase liquids (DNAPLs), Lightnon-aqueous phase liquids (LNAPLs) and heavy metals. They have becomethe top priority of groundwater contamination prevention and remediation.Thereby, perchloroethylene (PCE), benzene and hexavalent chromium (Cr~(6+))are chosed as target contaminants in the paper. In addition, with the rapiddevelopment of computer technology, numerical simulation has become animportant tool to study transport and remediation process of contaminant ingroundwater. Therefore, it is a very meaningful work about researchingtransport and remediation law of the three pollutants by numerical simulationtechnique.
Based on some groundwater remediation tests performed by our researchgroup in the past few years, we adhere to combination of self-developmentand introduction for groundwater numerical simulation software, and developprogram codes that can perform the following functions: multispecies mother-daughter kinetic reactions, Monod kinetics reactions, adsorption andchemical clogging of heavy metals. The program codes are on the basis ofMODFLOW-2005developed by USGS and MT3DMS developed by Prof.Chunmiao Zheng in University of Alabama. The main results can be writtenas follows.
For PCE-contaminated aquifer repaired by multi-PRB using iron andmicrobial community (FeMB) as reactive media, it built the multispeciesmother-daughter kinetic reactions model and developed its program codes.The results showed that (1) the bulk mass transfer coefficient was veryimportant for PCE transfering from non-aqueous phase to aqueous phase, andaffected the dissolution time and concentration peak,(2) thebiological/chemical reaction of PRB using FeMB as reactive media wasdominant in remediation process,(3) the concentration peak of two-stagePRB had a37%decrease comparing with that of one-stage, the value ofthree-stage had also a36%decrease comparing with that of two-stage,therefore multi-PRB could be a preferred option for intermediate products inremediation process,(4) the losses of reaction rate and hydraulic conductivitycan cause a decline of remediation effect.
For benzene-contaminzted aquifer repaired by slow-release oxygensource (SOS) technique and PRB with oxygen-releasing compounds (ORC),it built the Monod kinetics reactions model including benzene, DO andmicrobial species, and developed its program codes. The results showed that(1) placing the release oxygen well closer to source was more efficient,enough DO maybe accelerate the growth of microbial species which couldconsume more benzene,(2) the vertical velocity of gasoline in unsaturatedzone was dominates by its saturation, the most of gasoline was trapped byunsaturated zone after gasoline spills, it would cause potential risk of soilecological environment,(3) the scenario of oxygen-releasing rate15mg/Lcould have a80%decrease of benzene concentration in treated groundwater,the contaminant plume of benzene in saturated zone was near groundwatertable, it should be considered for PRB design,(4) the SOS and PRB with ORC were potential methods that can provide oxygen for groundwater.
For a column test of hexavalent chromium (Cr~(6+)), it developed aparameter estimation model for adsorption using genetic algorthms, thendesigned the PRB’s optimal size using modified chitosan (PEG-CTS#5) asreactive media. The results showed that (1) using MODFLOW/MT3DMS astool, the design method was appropriate on the based of the contaminantplume of0.1mg/L for Cr~(6+),(2) PEG-CTS#5may be a potential adsorptionmedium to restore Cr~(6+)-contaminated groundwater, but it would bulge ingroundwater and clog the flow,(3) the increase of horizontal and verticaltransverse dispersivity would decrease the PRB’s width and increase thelength and height, the heterogeneity was very important for PRB’s design.
For chemical clogging in groundwater remediation, it built a modelconsidering the chemical clogging around radial collector well, and developedits program codes. The results showed that (1) the model computing the waterdischarge of radial collector well was reasonable, the water discharge inbottom of horizontal screen lateral was bigger than that near the center of well,(2) the water discharge of radial collector well after45days declined by10-15%due to the chemical clogging, the groundwater table would raise andfinally influence engineering safety.
引文
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