表面活性剂强化地下水循环井技术修复NAPL污染含水层研究
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摘要
近年来地下水有机污染事件时有发生，特别是有机物的泄漏、随意排放等，严重的威胁了人类健康及社会安全，已经成为全球领域亟待解决的环境问题。
目前，针对地下水有机污染的修复技术较多，其中原位修复技术被认为是最有发展前景的修复技术。在众多的原位修复技术中，地下水循环井技术(groundwater circulation well, GCW)得到了快速发展，在国外已有上百个成功的场地修复实例，但在国内研究尚处于起步阶段，特别是对于循环井技术影响半径(radius of influence, ROI)的表征及影响因素的定量分析、有机物的浓度衰减规律、循环井修复区域的研究等，需要具体系统分析。针对NAPL普遍存在溶解度低的特点，表面活性剂强化修复技术(surfactant enhanced aquifer remednation,SEAR)被认为是提高有机物去除率最有效的原位修复技术之一，但目前该技术主要集中于机理及影响因素分析，且多为静态实验研究，对于动态冲洗过程中涉及到的影响因素等，尚需进一步深入研究。
针对以上存在的问题，本论文选用典型NAPL代表物苯、硝基苯和萘作为目标污染物，其中涵盖了LNAPL和DNAPL、挥发性和半挥发性有机物，本论文利用GCW和SEAR，单独进行NAPL污染含水层的修复实验，同时利用表面活性剂强化GCW修复效果，以期为地下水中挥发性和半挥发性有机物的去除提供新的途径。通过一系列模拟实验深入系统的研究了GCW的ROI估计及影响因素、GCW对有机物的修复效果、表面活性剂强化含水层修复效果及表面活性剂强化GCW等。论文取得的研究成果对于GCW技术的改进及其在地下水污染场地的实际应用具有重要的理论和实际意义。本论文的主要研究成果包括以下4个方面：
(1) GCW的ROI估计及影响因素
地下水循环井影响半径实验在二维模拟槽中进行，实验研究了地下水初始水位、曝气量、地下水初始流速和上下花管间距对ROI的影响，主要成果为：
①地下水初始水位主要影响临界曝气量及ROI。地下水初始水位越高，形成地下水循环的临界曝气量越小、ROI越大，但同时存在井内地下水水位上升过快、地下水由尾气口溢出情况，综合分析地下水初始水位定位45cm，即与循环井上部花管中间位置齐平。
②曝气量对ROI影响较小；随着曝气量提高，∑△h值显著增加，但曝气量上升至0.7m~3/h后，∑△h变化不再明显，综合确定曝气量为0.7m~3/h。
③地下水初始流速在0.1~1.0m/d范围内，几乎不影响ROI，但∑△h较静水条件下略有上升，实验结论表明地下水初始流速影响基本可忽略不计。
④上下花管间距对ROI影响不大，但间距变大增强了地下水循环流速，结论说明循环井结构主要影响地下水循环强度。
⑤实验过程中发现，各测压管内水位高度变化迅速并能较快达到平衡，说明循环井能够快速启动、稳定运行。
(2) GCW修复NAPL污染含水层
循环井技术修复NAPL污染含水层实验也在二维模拟槽中进行，实验分析了苯、硝基苯和萘的迁移规律及循环井的修复效果，具体研究成果为：
①苯、硝基苯和萘在实验介质上的吸附均满足线性吸附，吸附系数受有机物性质、介质粒径及介质有机质含量影响，其中有机质含量影响程度大于介质粒径。
②有机物在地下水中同时发生水平和垂向迁移，以硝基苯的垂向迁移最为明显，萘的迁移具有明显滞后性，污染第50d后，整个模拟槽被全部污染。
③靠近循环井的有机物被优先去除，并逐渐形成一个以循环井为轴的锥形修复区域。苯的修复效果良好，累积曝气14h后，地下水中已基本检测不到苯，但硝基苯和萘的去除明显具有拖尾现象，拖尾浓度分别为71.19mg/L和1.82mg/L。循环井修复效果受有机物挥发性和迁移性综合影响。
④硝基苯和萘相对浓度在0~0.5范围内时，C/Co与S/So近似线性正相关，可以大致估算不同修复程度下循环井的相对修复区域。
(3)表面活性剂强化NAPL污染含水层修复
①基于表面活性剂增溶和增流的修复机理，初步选用阴离子型表面活性剂SDBS和非离子型表面活性剂Tween80，从吸附性、降低表面张力能力和增溶性能3个方面进行考察，综合对比选用Tween80作为强化表面活性剂。
②Tween80修复NAPL污染含水层的冲洗浓度应大于2.0g/L；实验中存在最佳表面活性剂冲洗浓度10.0g/L和最佳冲洗流速3.0mL/min。
③实验中发现，介质粒径较细，存在轻微阻塞现象，此时应适当降低表面活性剂浓度；介质粒径较粗时，存在表面活性剂优先纵向迁移问题，此时应适当减缓冲洗流速。
④有机质含量(15.67%)较高的介质，苯、硝基苯和萘的去除严重受阻，累积去除率不足50%，表面活性剂强化修复技术不再适用。
(4)表面活性剂强化GCW修复NAPL污染含水层
针对循环井技术单独运行时，存在硝基苯和萘的浓度拖尾现象，利用Tween80溶液进行强化修复。
①Tween80溶液进入地下水后，纵向迁移距离明显大于横向迁移；不同曝气时间下，浓度均大于2.0g/L的区域基本固定在循环井两侧，没有发生明显的扩散现象，实验结论表明循环井可以有效控制Tween80的水力迁移。
②Tween80溶液提高了硝基苯和萘的水相溶解度，平均浓度分别为147.07mg/L和3.62mg/L，但明显小于静态增溶数据。实验结果说明，增溶效果不仅受表面活性剂和有机物性质影响，同时也受环境介质影响。
③硝基苯和萘的修复效果均有显著提高，累积曝气14h后，拖尾浓度分别下降至41.43mg/L和0.69mg/L，明显小于GCW单独使用时的拖尾浓度，说明表面活性剂对循环井技术具有很好的强化效果。
④硝基苯的衰减系数大于萘，但两者与循环井的相对位置均呈现两边高、中间低的趋势，实验结论说明，表面活性剂的注入提高了有机物的迁移性，此时循环井修复效果主要受有机物挥发性影响。
⑤硝基苯和萘相对浓度在0~0.5范围内时，随着C/Co减小，S/So呈缓慢下降，说明表面活性剂提高了循环井的修复区域。
In recent years, groundwater organic pollution incidents are frequently occurredin china especially duing to the waste leakage, discharge and explosion, and havebecome the urgent problems in the environmental domain. Groundwater circulationwell is a effective mean to removal volatile organic compounds and has been proveneffective in the processing of field remediation application. However, the study ofGCW has just began in china, and ROI (radius of influence) representation andrelated influencing factors, concentration attenuation of organic compounds as wellas the zone of influencing are all needed to study systematically. In the light of thelow aqueous solubility of NAPL (Non Aqueous Phase Liquids), surfactant-enhancedaquifer remediation is considered to be the most effective in situ remediationtechnology. In the past research, most studies focused on the mechanism study, whilethe dynamic flushing process needs further research.
According to the previous studies, benzene, nitrobenzene and naphthalene werechosen as the typical NAPLs, and the remediation effect of contaminated aquiferwith surfactant enhanced groundwater circulation well was carried out. A series ofsimulations experiments were conducted to investgate: radius of influence of GCWand the influencing factors, such as groundwater initial level, aeration rate,groundwater velocity and structure of GCW; the effect of GCW, including thesorption of organic compounds on different experimental medium, concentrationattenuation of contaminants in the process of CGW and the zone of influence ofGCW; the effect of SEAR, including: the surfactant selection, the critical flushingconcentration as well as the influencing factors; surfactant-enhanced GCW, including the hydraulic control of surfactant by GCW, the surfactant sulibilozaiton,concentration attenuation of organic compounds and the zone of influence.
A two-dimensional sand tank was used to identified the ZOI of GCW, the effectof influencing factors, such as groundwater initial level, aeration rate, groundwatervelocity and structure of GCW were all studied, the results demonstrate that:(1)maximum horizontal distance of the zone that water level change can be defined asthe ROI of GCW;(2) the higher of the initial groundwater level, the smaller of thecritical aeration rate and the stronger of the ciucuration of groundwater.(3) aerationrate was positive to∑△h, but has litter influence on ROI.(4) A slight increment of∑△h was observed when the groundwater flow velocity increased from0.1to1.0m/d, but the ROI was basically stable at60cm.(5) The groundwater circulation flowvelocity increased with the increment of the distance between upper and bottom tube,and the highest circulation velocity was up to28.60m/d.
The remediation of NAPL contaminated aquifer by GCW was carried out in atwo-dimension sand tank. The mainly experimental results are:(1) the sorptionisotherm of benzene, nitrobenzene and naphthalene were linear models and theadsorption coefficient was affected by medium size and organic matter content.(2)The preferentially lateral was observed when organic compounds leaked intogroundwater as well as the longitudinal concentration diffusion, the time thatbenzene, nitrobenzene and naphthalene polluted the whole sand tank were30d,30dand50d, respectively.(3) After accumulated aeration time exceeded14h, benzenecan not be detectived in the groundwater, whereas the remove of nitrobenzene andnaphthalene entered the stage of tail and the tail concentration were71.19mg/L and1.82mg/L, respectively.(4) The relative average concentration of organic matter ineach column was negative to the log of the accumulated aeration time; concentrationattenuation of each column was decreased with the increment of the distancebetween each column and the GCW; benzene attenuation coefficient was higher thannitrobenzene and naphthalene.(5) The position of nitrobenzene and naphthaleneconcentration dropped fastest located in the left of the sand tank, and the S/Sowaspositive to the C/Cowhen C/Coof nitrobenzene and naphthalene ranged from0to 0.5.
According to the mechanism of solubilization and mobilization, SDBS andTween80were selected and the investigation of sorption, lowering the surfacetension and solibilizaiton properties were carried out.(1) The sorption isotherms ofSDBS and Tween80in the medium sand were Langmiur model and Frundlich model,respectively. The highest saturated adsorption amounts were2.04and7.87mg/g.(2)the capability of reduce surface tension of Tween80was superior to SDBS.(3) Kmcof benzene, nitrobenzene and naphthalene in Tween80solution were4.44×103,4.38×103and1.52×103mL/g, that greater than Kmcin the SDBS solution.(4)Temperature and ion strength were positive to the solubilization of naphthalene inTween80solution, and the higher of the Tween80solution concentration, the greaterof the naphthalene apparent solubility.
A one-dimension columns were utilized to study benzene, nitrobenzene andnaphthalene removal efficiency in groundwater with surfactant flushing, the mainresults are:(1) The critical flushing concentration of Tween80was2.0g/L.(2) Theremoval efficiency was increased by the increment of Tween80solutionconcentration, but the removal efficiency increase was not significant once theTween80solution concentration exceeded10.0g/L.(3) The removal efficiency canbe imporved with the increase of flushing velocity, but too higher flushing velocitymay decrease the removal efficiency.(4) Medium size has great effect on theremoval efficiency. Too small or to large size of the medium would both notconducive to the removal of organic matter.(5) Surfactant enhanced aquiferremediation would be not appropriate when the organic matter content was toohigher.
According to the residual concentration of nitrobenzene and naphthalene,Tween80solution was used to enhance the removal efficiency of GCW. The mainresults are:(1) the preferentially longitudinal of Tween80solution was observed aswell as the lateral concentration diffusion.(2) The migration of Tween80in theaquifer can be controlled by GCW; Tween80concentration that higher than2.0g/L,which covered an area of more than80%of the contaminated aera distributed evently on both sides of GCW after aeration time exceeded14h.(3) Nitrobenzeneand naphthalene concentration in aqueous were greatly increased by surfactantsolubilization and the average concentration were up to147.07mg/L and3.62mg/L,but lower than solibilizaiton experimental results. The tail concentration ofnireobenzene and naphthalene decreased to41.43mg/L and0.69mg/L after aeration14h.(4) Concentration attenuation of nitrobenzene and naphthalene in each columnwas negative to the log of accumulated aeration time, and naphthalene concentrationattenuation was higher than naphthalene.(5) The position that nitrobenzene andnaphthalene concentration dropped fastest in the middle of the sand tank, and C/Cowas positive to S/Soas C/Corange from0to0.5.
目前，针对地下水有机污染的修复技术较多，其中原位修复技术被认为是最有发展前景的修复技术。在众多的原位修复技术中，地下水循环井技术(groundwater circulation well, GCW)得到了快速发展，在国外已有上百个成功的场地修复实例，但在国内研究尚处于起步阶段，特别是对于循环井技术影响半径(radius of influence, ROI)的表征及影响因素的定量分析、有机物的浓度衰减规律、循环井修复区域的研究等，需要具体系统分析。针对NAPL普遍存在溶解度低的特点，表面活性剂强化修复技术(surfactant enhanced aquifer remednation,SEAR)被认为是提高有机物去除率最有效的原位修复技术之一，但目前该技术主要集中于机理及影响因素分析，且多为静态实验研究，对于动态冲洗过程中涉及到的影响因素等，尚需进一步深入研究。
针对以上存在的问题，本论文选用典型NAPL代表物苯、硝基苯和萘作为目标污染物，其中涵盖了LNAPL和DNAPL、挥发性和半挥发性有机物，本论文利用GCW和SEAR，单独进行NAPL污染含水层的修复实验，同时利用表面活性剂强化GCW修复效果，以期为地下水中挥发性和半挥发性有机物的去除提供新的途径。通过一系列模拟实验深入系统的研究了GCW的ROI估计及影响因素、GCW对有机物的修复效果、表面活性剂强化含水层修复效果及表面活性剂强化GCW等。论文取得的研究成果对于GCW技术的改进及其在地下水污染场地的实际应用具有重要的理论和实际意义。本论文的主要研究成果包括以下4个方面：
(1) GCW的ROI估计及影响因素
地下水循环井影响半径实验在二维模拟槽中进行，实验研究了地下水初始水位、曝气量、地下水初始流速和上下花管间距对ROI的影响，主要成果为：
①地下水初始水位主要影响临界曝气量及ROI。地下水初始水位越高，形成地下水循环的临界曝气量越小、ROI越大，但同时存在井内地下水水位上升过快、地下水由尾气口溢出情况，综合分析地下水初始水位定位45cm，即与循环井上部花管中间位置齐平。
②曝气量对ROI影响较小；随着曝气量提高，∑△h值显著增加，但曝气量上升至0.7m~3/h后，∑△h变化不再明显，综合确定曝气量为0.7m~3/h。
③地下水初始流速在0.1~1.0m/d范围内，几乎不影响ROI，但∑△h较静水条件下略有上升，实验结论表明地下水初始流速影响基本可忽略不计。
④上下花管间距对ROI影响不大，但间距变大增强了地下水循环流速，结论说明循环井结构主要影响地下水循环强度。
⑤实验过程中发现，各测压管内水位高度变化迅速并能较快达到平衡，说明循环井能够快速启动、稳定运行。
(2) GCW修复NAPL污染含水层
循环井技术修复NAPL污染含水层实验也在二维模拟槽中进行，实验分析了苯、硝基苯和萘的迁移规律及循环井的修复效果，具体研究成果为：
①苯、硝基苯和萘在实验介质上的吸附均满足线性吸附，吸附系数受有机物性质、介质粒径及介质有机质含量影响，其中有机质含量影响程度大于介质粒径。
②有机物在地下水中同时发生水平和垂向迁移，以硝基苯的垂向迁移最为明显，萘的迁移具有明显滞后性，污染第50d后，整个模拟槽被全部污染。
③靠近循环井的有机物被优先去除，并逐渐形成一个以循环井为轴的锥形修复区域。苯的修复效果良好，累积曝气14h后，地下水中已基本检测不到苯，但硝基苯和萘的去除明显具有拖尾现象，拖尾浓度分别为71.19mg/L和1.82mg/L。循环井修复效果受有机物挥发性和迁移性综合影响。
④硝基苯和萘相对浓度在0~0.5范围内时，C/Co与S/So近似线性正相关，可以大致估算不同修复程度下循环井的相对修复区域。
(3)表面活性剂强化NAPL污染含水层修复
①基于表面活性剂增溶和增流的修复机理，初步选用阴离子型表面活性剂SDBS和非离子型表面活性剂Tween80，从吸附性、降低表面张力能力和增溶性能3个方面进行考察，综合对比选用Tween80作为强化表面活性剂。
②Tween80修复NAPL污染含水层的冲洗浓度应大于2.0g/L；实验中存在最佳表面活性剂冲洗浓度10.0g/L和最佳冲洗流速3.0mL/min。
③实验中发现，介质粒径较细，存在轻微阻塞现象，此时应适当降低表面活性剂浓度；介质粒径较粗时，存在表面活性剂优先纵向迁移问题，此时应适当减缓冲洗流速。
④有机质含量(15.67%)较高的介质，苯、硝基苯和萘的去除严重受阻，累积去除率不足50%，表面活性剂强化修复技术不再适用。
(4)表面活性剂强化GCW修复NAPL污染含水层
针对循环井技术单独运行时，存在硝基苯和萘的浓度拖尾现象，利用Tween80溶液进行强化修复。
①Tween80溶液进入地下水后，纵向迁移距离明显大于横向迁移；不同曝气时间下，浓度均大于2.0g/L的区域基本固定在循环井两侧，没有发生明显的扩散现象，实验结论表明循环井可以有效控制Tween80的水力迁移。
②Tween80溶液提高了硝基苯和萘的水相溶解度，平均浓度分别为147.07mg/L和3.62mg/L，但明显小于静态增溶数据。实验结果说明，增溶效果不仅受表面活性剂和有机物性质影响，同时也受环境介质影响。
③硝基苯和萘的修复效果均有显著提高，累积曝气14h后，拖尾浓度分别下降至41.43mg/L和0.69mg/L，明显小于GCW单独使用时的拖尾浓度，说明表面活性剂对循环井技术具有很好的强化效果。
④硝基苯的衰减系数大于萘，但两者与循环井的相对位置均呈现两边高、中间低的趋势，实验结论说明，表面活性剂的注入提高了有机物的迁移性，此时循环井修复效果主要受有机物挥发性影响。
⑤硝基苯和萘相对浓度在0~0.5范围内时，随着C/Co减小，S/So呈缓慢下降，说明表面活性剂提高了循环井的修复区域。
In recent years, groundwater organic pollution incidents are frequently occurredin china especially duing to the waste leakage, discharge and explosion, and havebecome the urgent problems in the environmental domain. Groundwater circulationwell is a effective mean to removal volatile organic compounds and has been proveneffective in the processing of field remediation application. However, the study ofGCW has just began in china, and ROI (radius of influence) representation andrelated influencing factors, concentration attenuation of organic compounds as wellas the zone of influencing are all needed to study systematically. In the light of thelow aqueous solubility of NAPL (Non Aqueous Phase Liquids), surfactant-enhancedaquifer remediation is considered to be the most effective in situ remediationtechnology. In the past research, most studies focused on the mechanism study, whilethe dynamic flushing process needs further research.
According to the previous studies, benzene, nitrobenzene and naphthalene werechosen as the typical NAPLs, and the remediation effect of contaminated aquiferwith surfactant enhanced groundwater circulation well was carried out. A series ofsimulations experiments were conducted to investgate: radius of influence of GCWand the influencing factors, such as groundwater initial level, aeration rate,groundwater velocity and structure of GCW; the effect of GCW, including thesorption of organic compounds on different experimental medium, concentrationattenuation of contaminants in the process of CGW and the zone of influence ofGCW; the effect of SEAR, including: the surfactant selection, the critical flushingconcentration as well as the influencing factors; surfactant-enhanced GCW, including the hydraulic control of surfactant by GCW, the surfactant sulibilozaiton,concentration attenuation of organic compounds and the zone of influence.
A two-dimensional sand tank was used to identified the ZOI of GCW, the effectof influencing factors, such as groundwater initial level, aeration rate, groundwatervelocity and structure of GCW were all studied, the results demonstrate that:(1)maximum horizontal distance of the zone that water level change can be defined asthe ROI of GCW;(2) the higher of the initial groundwater level, the smaller of thecritical aeration rate and the stronger of the ciucuration of groundwater.(3) aerationrate was positive to∑△h, but has litter influence on ROI.(4) A slight increment of∑△h was observed when the groundwater flow velocity increased from0.1to1.0m/d, but the ROI was basically stable at60cm.(5) The groundwater circulation flowvelocity increased with the increment of the distance between upper and bottom tube,and the highest circulation velocity was up to28.60m/d.
The remediation of NAPL contaminated aquifer by GCW was carried out in atwo-dimension sand tank. The mainly experimental results are:(1) the sorptionisotherm of benzene, nitrobenzene and naphthalene were linear models and theadsorption coefficient was affected by medium size and organic matter content.(2)The preferentially lateral was observed when organic compounds leaked intogroundwater as well as the longitudinal concentration diffusion, the time thatbenzene, nitrobenzene and naphthalene polluted the whole sand tank were30d,30dand50d, respectively.(3) After accumulated aeration time exceeded14h, benzenecan not be detectived in the groundwater, whereas the remove of nitrobenzene andnaphthalene entered the stage of tail and the tail concentration were71.19mg/L and1.82mg/L, respectively.(4) The relative average concentration of organic matter ineach column was negative to the log of the accumulated aeration time; concentrationattenuation of each column was decreased with the increment of the distancebetween each column and the GCW; benzene attenuation coefficient was higher thannitrobenzene and naphthalene.(5) The position of nitrobenzene and naphthaleneconcentration dropped fastest located in the left of the sand tank, and the S/Sowaspositive to the C/Cowhen C/Coof nitrobenzene and naphthalene ranged from0to 0.5.
According to the mechanism of solubilization and mobilization, SDBS andTween80were selected and the investigation of sorption, lowering the surfacetension and solibilizaiton properties were carried out.(1) The sorption isotherms ofSDBS and Tween80in the medium sand were Langmiur model and Frundlich model,respectively. The highest saturated adsorption amounts were2.04and7.87mg/g.(2)the capability of reduce surface tension of Tween80was superior to SDBS.(3) Kmcof benzene, nitrobenzene and naphthalene in Tween80solution were4.44×103,4.38×103and1.52×103mL/g, that greater than Kmcin the SDBS solution.(4)Temperature and ion strength were positive to the solubilization of naphthalene inTween80solution, and the higher of the Tween80solution concentration, the greaterof the naphthalene apparent solubility.
A one-dimension columns were utilized to study benzene, nitrobenzene andnaphthalene removal efficiency in groundwater with surfactant flushing, the mainresults are:(1) The critical flushing concentration of Tween80was2.0g/L.(2) Theremoval efficiency was increased by the increment of Tween80solutionconcentration, but the removal efficiency increase was not significant once theTween80solution concentration exceeded10.0g/L.(3) The removal efficiency canbe imporved with the increase of flushing velocity, but too higher flushing velocitymay decrease the removal efficiency.(4) Medium size has great effect on theremoval efficiency. Too small or to large size of the medium would both notconducive to the removal of organic matter.(5) Surfactant enhanced aquiferremediation would be not appropriate when the organic matter content was toohigher.
According to the residual concentration of nitrobenzene and naphthalene,Tween80solution was used to enhance the removal efficiency of GCW. The mainresults are:(1) the preferentially longitudinal of Tween80solution was observed aswell as the lateral concentration diffusion.(2) The migration of Tween80in theaquifer can be controlled by GCW; Tween80concentration that higher than2.0g/L,which covered an area of more than80%of the contaminated aera distributed evently on both sides of GCW after aeration time exceeded14h.(3) Nitrobenzeneand naphthalene concentration in aqueous were greatly increased by surfactantsolubilization and the average concentration were up to147.07mg/L and3.62mg/L,but lower than solibilizaiton experimental results. The tail concentration ofnireobenzene and naphthalene decreased to41.43mg/L and0.69mg/L after aeration14h.(4) Concentration attenuation of nitrobenzene and naphthalene in each columnwas negative to the log of accumulated aeration time, and naphthalene concentrationattenuation was higher than naphthalene.(5) The position that nitrobenzene andnaphthalene concentration dropped fastest in the middle of the sand tank, and C/Cowas positive to S/Soas C/Corange from0to0.5.
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