土壤通气—微生物降解耦合修复现场石油烃污染土壤研究
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摘要
污染土壤的微生物修复技术具有费用低、处理效果好、无二次污染等优点，可用于被石油烃、重金属等污染物污染的土壤治理，但该技术存在修复周期长和特定高效降解菌难以获得等不利因素。土壤通气（Soil Venting，SV）技术是用于修复不饱和区域土壤中挥发性有机物的新兴修复技术，该技术包括土壤气相抽提（Soil Vapor Extraction，SVE）及其衍生技术如生物通风技术（Bioventing，BV）等，土壤通气技术对于土壤渗透性要求较高并且后期存在拖尾效应。实际修复工程中单一修复技术往往不能解决土壤的石油烃污染问题，因此对土壤通气（SVE/BV）-微生物降解耦合修复技术进行深入研究是十分必要的。
对来自辽河油田污泥和天津开发区某现场被轻质油污染的土壤中的微生物进行了筛选、分离，得到了四株能够对原油和轻质油降解的高效微生物菌株，并确定了优势菌种适宜的生长条件。同时对石油降解菌株固定化载体的选择进行研究，综合考虑载体的吸菌量、持水能力及密度等特性，确定了实验条件下固态菌剂的最佳载体。
以天津开发区现场具有代表性的粘性土壤-淤泥质粉质粘土夹粉砂为研究对象，通过吸附平衡实验和原油降解实验探讨了该类型土壤对原油的吸附性能以及高效石油降解菌对该土壤中原油的降解规律。通过吸附实验确定吸附常数等参数，探讨原油在土壤中的吸附机理。采用生物泥浆法考察了原油在现场粘性土壤中的降解规律，并且对一级降解动力学模型进行了改进。本文同时考察了表面活性剂对土壤中原油降解的影响，发现鼠李糖脂在降解初期能明显促进土壤中原油的降解。
基于高效石油降解菌剂的自然通风技术在辽河油田的应用研究中，采用土壤自然通风（辅助以定期深翻）-微生物降解的异位修复方法，验证了添加微生物菌剂在油田油泥中的应用效果，该固态菌剂对土壤中原油的降解效果明显优于自然降解。现场试验条件下，微生物生长相对生长缓慢，仍符合一级生长动力学，但没有明显的延迟期及对数生长期等阶段。
在天津开发区某轻质油污染场地建立原位修复试验体系，系统地研究了挥发性石油烃的土壤通气（SVE/BV）-微生物降解耦合修复的机理。单井稳态抽气试验，确定了SVE/BV过程的气相压力分布、不饱和区域土壤（粘性土壤）的空气渗透率、压力影响半径等重要参数。现场优势土著微生物（细菌）的原位自然驯化阶段（1~140天），考察了土壤含水量、 pH值以及土壤环境温度等因素对微生物生长的影响。
现场条件下，土壤中挥发性石油烃（异辛烷）的去除经历了105天，以土壤通气开始时间为节点，划分为单纯微生物降解（33~132天）和土壤通气（SVE/BV）-微生物降解耦合过程（133~138天）两个阶段。通过单纯微生物降解试验，获得了生物降解动力学模型参数；通过单井稳态土壤通气试验研究了抽提尾气中的污染物去除机制，尾气中的异辛烷的去除符合幂函数关系。顶空法测定土壤固相中污染物（异辛烷）的初始质量百分比含量为0.30％，单纯生物降解阶段污染物的去除率为63.33％，而土壤通气（SVE/BV）-微生物降解耦合修复过程污染物的去除率达到了72.73％。现场试验证明采用土壤通气（SVE/BV）-微生物降解耦合修复技术，可有效去除不饱和区域土壤中的挥发性石油烃。
在对土壤通气的气相流动方程和石油烃污染土壤微生物降解模型分析的基础上，提出了挥发性石油烃的土壤通气（SVE/BV）-微生物降解耦合修复传质模型，并对单井抽气系统的稳态流场下的传质模型进行了求解。模拟污染物（异辛烷）去除的模型计算结果与现场数据基本吻合，说明本文提出的数学模型能够对现场土壤通气-微生物修复过程进行正确预测。
本文研究成果，特别是挥发性石油烃的原位土壤通气（SVE/BV）-微生物降解耦合修复的试验和理论研究成果可作为土壤修复中试或现场修复的基础数据和参考依据。
Microbial remediation technology of contaminated soil has the advantages oflow expense, high efficiency, and no secondary condamination, et al. So thistechnology could be used to treat the soil which is been contaminated by theprtroleum hydrocarbons, and the heavy metals, et al. But this technology also has thedisadvantages of long remediation circles and the requirement of specific excellentdegrading bacteria which is difficult to get. Soil Venting (SV) is gaining acceptance asa remediation technology for unsaturated soils contaminated with volatile organiccompounds (VOCs). This technology includes the technology of Soil VaporExtraction (SVE), and the technology of Bioventing (BV) which is derived from theSVE technology, etc. But the application of the SVE technology requires the highpermeability of the contaminated soil that is treated, and also this technology has taileffect. In the engineering project, the single remediation technology for thecontaminated soil is actually not enough to solve the problem of soil contaminationwith petroleum hydrocarbons completely. So the in-depth research on the couplingtechnology of SVE/BV technology and microbial remediation technology is verynecessary.
In this work, the microorganisms existing in the heavily contaminated soil fromLiaohe Oil Field and the lightly contaminated soil from some field of TEDA (TianjinEconomy and Development Area) was isolated and screened out. Four types of highperformance microbial bacteria which could be used to degrade the crude oil and lightoil was obtained. The suitable growth conditions for these dominant microbialbacteria were determined. Research on the selection of immobilized carriers for thesemicrobial bacteria was also conducted. In this research, the properties of bacteriaadsorption quantity, moisture performance, density of the immobilized carriers wereconsidered. So the best carrier for the soild bacteria under the experimental conditionswas determined.
Using the typical silty clay from the TEDA field, the crude oil adsorptionperformance of this type of soil and the performance of crude oil biodegradation withthe dominant microbial bacteria was discussed via the crude oil adsorptionexperiments and the crude oil biodegradation experiments. The mechanism of theadsorption of crude oil in the soil and the parameters such as adsorption constants was determined with the crude oil adsorption equilibrium experiment. Using the biologicalmud method, the performance of the bidegradation of crude oil in the silty clay wasdetermined, and the first-order’s bidegradation kinetic model was corrected. Theboosting effect of surfactant on the biodegradation of crude oil in the soil was alsoobserved in this work. And it was found that the rhamnolipid could greatly acceleratethe rate of degradation of crude oil in the soil especially at the beginning ofbiodegradation. In the field application research of high performance petroleumhydrocarbons degradation soild bacteria, the good effect of microbial solid bacteria inthe treatment of oil soil from the Liaohe Oil Field was validated using the biodegradationoff-situ remediation approach of natural ventilation (with the timely excavation for thesoil) technology, so these microbial bacteria appears obvious advantages over thenatural degradation when used to treat the crude oil in the soil.
The in-situ remediation experimental equipment system was set up in a TEDAfield which was lightly contaminated by light oil. Using this experimental equipmentsystem, the coupling treatment mechanism of in-situ microbial remediation andSVE/BV for the volatile petroleum hydrocarbons was systemically observed. Theimportant parameters such as the vapor pressure distribution, air permeability ofunsaturated area soil (silty clay), and the pressure influnce radius was determined viathe single steady state extracting experiments and the air respiration test.
During the phase of in-situ natural domestication of the field dominant nativemicrobial bacteria, the effect of important factors such as soil moisture, pH value, andthe soil temperature on the growth of microbial bacteria were observed. Under thefield conditions, the treatment of volatile petroleum hydrocarbons (isooctane) in thesoil spanned about105days, with the boundary point marked by the start time ofSVE/BV, this could be divided to be the biodegradation stage（from33to132days）and the the coupling SVE/BV and microbial remediation stag（efrom133to138days）.Using the experimental data from the biodegradation experiments, the degradationkinetic model parameters were obtained. The removal mechanism of contaminants inthe extraction emissions was studied via the single steady state soil extractingexperiments, and it was found that the removal of isooctane in the extractionemissions in the terms of time agreed well with the power function. The initial massweight of contaminant isooctane in the soil solid phase measured with the headspaceanalysis method was0.30%, and the contaminant removed percent at the end of thefirst stage was63.33%, while the contaminant removed percent at the end of the second stage was72.73％. The great performance of the coupling SVE/BV andmicrobial remediation technology that was applied to remove the volatile petroleumhydrocarbons was validated by the field experiments.
Based on the equation of vapor flow of SVE/BV and the analysis of thebiodegradation kinetic model for the contaminated soil with petroleum, the masstransfer model of the coupling SVE/BV and microbial remediation for the treatmentof volatile petroleum hydrocarbons was proposed. Under steady state conditions, thecalculation results of the model of the single component and single extraction wellsystem agreed well with the field data, so the mathematical model that proposed inthis dissertation could be used to provide accurate data for the SVE/BV and microbialremediation treatment of field soil.
The research results of this dissertation, especially the experimental andtheoretical conclusions of the research of the SVE/BV and microbial remediationin-situ treatment of volatile petroleum hydrocarbons, could be used as the basic dataand the reference for the pilot or field treatment of contaminated soil.
对来自辽河油田污泥和天津开发区某现场被轻质油污染的土壤中的微生物进行了筛选、分离，得到了四株能够对原油和轻质油降解的高效微生物菌株，并确定了优势菌种适宜的生长条件。同时对石油降解菌株固定化载体的选择进行研究，综合考虑载体的吸菌量、持水能力及密度等特性，确定了实验条件下固态菌剂的最佳载体。
以天津开发区现场具有代表性的粘性土壤-淤泥质粉质粘土夹粉砂为研究对象，通过吸附平衡实验和原油降解实验探讨了该类型土壤对原油的吸附性能以及高效石油降解菌对该土壤中原油的降解规律。通过吸附实验确定吸附常数等参数，探讨原油在土壤中的吸附机理。采用生物泥浆法考察了原油在现场粘性土壤中的降解规律，并且对一级降解动力学模型进行了改进。本文同时考察了表面活性剂对土壤中原油降解的影响，发现鼠李糖脂在降解初期能明显促进土壤中原油的降解。
基于高效石油降解菌剂的自然通风技术在辽河油田的应用研究中，采用土壤自然通风（辅助以定期深翻）-微生物降解的异位修复方法，验证了添加微生物菌剂在油田油泥中的应用效果，该固态菌剂对土壤中原油的降解效果明显优于自然降解。现场试验条件下，微生物生长相对生长缓慢，仍符合一级生长动力学，但没有明显的延迟期及对数生长期等阶段。
在天津开发区某轻质油污染场地建立原位修复试验体系，系统地研究了挥发性石油烃的土壤通气（SVE/BV）-微生物降解耦合修复的机理。单井稳态抽气试验，确定了SVE/BV过程的气相压力分布、不饱和区域土壤（粘性土壤）的空气渗透率、压力影响半径等重要参数。现场优势土著微生物（细菌）的原位自然驯化阶段（1~140天），考察了土壤含水量、 pH值以及土壤环境温度等因素对微生物生长的影响。
现场条件下，土壤中挥发性石油烃（异辛烷）的去除经历了105天，以土壤通气开始时间为节点，划分为单纯微生物降解（33~132天）和土壤通气（SVE/BV）-微生物降解耦合过程（133~138天）两个阶段。通过单纯微生物降解试验，获得了生物降解动力学模型参数；通过单井稳态土壤通气试验研究了抽提尾气中的污染物去除机制，尾气中的异辛烷的去除符合幂函数关系。顶空法测定土壤固相中污染物（异辛烷）的初始质量百分比含量为0.30％，单纯生物降解阶段污染物的去除率为63.33％，而土壤通气（SVE/BV）-微生物降解耦合修复过程污染物的去除率达到了72.73％。现场试验证明采用土壤通气（SVE/BV）-微生物降解耦合修复技术，可有效去除不饱和区域土壤中的挥发性石油烃。
在对土壤通气的气相流动方程和石油烃污染土壤微生物降解模型分析的基础上，提出了挥发性石油烃的土壤通气（SVE/BV）-微生物降解耦合修复传质模型，并对单井抽气系统的稳态流场下的传质模型进行了求解。模拟污染物（异辛烷）去除的模型计算结果与现场数据基本吻合，说明本文提出的数学模型能够对现场土壤通气-微生物修复过程进行正确预测。
本文研究成果，特别是挥发性石油烃的原位土壤通气（SVE/BV）-微生物降解耦合修复的试验和理论研究成果可作为土壤修复中试或现场修复的基础数据和参考依据。
Microbial remediation technology of contaminated soil has the advantages oflow expense, high efficiency, and no secondary condamination, et al. So thistechnology could be used to treat the soil which is been contaminated by theprtroleum hydrocarbons, and the heavy metals, et al. But this technology also has thedisadvantages of long remediation circles and the requirement of specific excellentdegrading bacteria which is difficult to get. Soil Venting (SV) is gaining acceptance asa remediation technology for unsaturated soils contaminated with volatile organiccompounds (VOCs). This technology includes the technology of Soil VaporExtraction (SVE), and the technology of Bioventing (BV) which is derived from theSVE technology, etc. But the application of the SVE technology requires the highpermeability of the contaminated soil that is treated, and also this technology has taileffect. In the engineering project, the single remediation technology for thecontaminated soil is actually not enough to solve the problem of soil contaminationwith petroleum hydrocarbons completely. So the in-depth research on the couplingtechnology of SVE/BV technology and microbial remediation technology is verynecessary.
In this work, the microorganisms existing in the heavily contaminated soil fromLiaohe Oil Field and the lightly contaminated soil from some field of TEDA (TianjinEconomy and Development Area) was isolated and screened out. Four types of highperformance microbial bacteria which could be used to degrade the crude oil and lightoil was obtained. The suitable growth conditions for these dominant microbialbacteria were determined. Research on the selection of immobilized carriers for thesemicrobial bacteria was also conducted. In this research, the properties of bacteriaadsorption quantity, moisture performance, density of the immobilized carriers wereconsidered. So the best carrier for the soild bacteria under the experimental conditionswas determined.
Using the typical silty clay from the TEDA field, the crude oil adsorptionperformance of this type of soil and the performance of crude oil biodegradation withthe dominant microbial bacteria was discussed via the crude oil adsorptionexperiments and the crude oil biodegradation experiments. The mechanism of theadsorption of crude oil in the soil and the parameters such as adsorption constants was determined with the crude oil adsorption equilibrium experiment. Using the biologicalmud method, the performance of the bidegradation of crude oil in the silty clay wasdetermined, and the first-order’s bidegradation kinetic model was corrected. Theboosting effect of surfactant on the biodegradation of crude oil in the soil was alsoobserved in this work. And it was found that the rhamnolipid could greatly acceleratethe rate of degradation of crude oil in the soil especially at the beginning ofbiodegradation. In the field application research of high performance petroleumhydrocarbons degradation soild bacteria, the good effect of microbial solid bacteria inthe treatment of oil soil from the Liaohe Oil Field was validated using the biodegradationoff-situ remediation approach of natural ventilation (with the timely excavation for thesoil) technology, so these microbial bacteria appears obvious advantages over thenatural degradation when used to treat the crude oil in the soil.
The in-situ remediation experimental equipment system was set up in a TEDAfield which was lightly contaminated by light oil. Using this experimental equipmentsystem, the coupling treatment mechanism of in-situ microbial remediation andSVE/BV for the volatile petroleum hydrocarbons was systemically observed. Theimportant parameters such as the vapor pressure distribution, air permeability ofunsaturated area soil (silty clay), and the pressure influnce radius was determined viathe single steady state extracting experiments and the air respiration test.
During the phase of in-situ natural domestication of the field dominant nativemicrobial bacteria, the effect of important factors such as soil moisture, pH value, andthe soil temperature on the growth of microbial bacteria were observed. Under thefield conditions, the treatment of volatile petroleum hydrocarbons (isooctane) in thesoil spanned about105days, with the boundary point marked by the start time ofSVE/BV, this could be divided to be the biodegradation stage（from33to132days）and the the coupling SVE/BV and microbial remediation stag（efrom133to138days）.Using the experimental data from the biodegradation experiments, the degradationkinetic model parameters were obtained. The removal mechanism of contaminants inthe extraction emissions was studied via the single steady state soil extractingexperiments, and it was found that the removal of isooctane in the extractionemissions in the terms of time agreed well with the power function. The initial massweight of contaminant isooctane in the soil solid phase measured with the headspaceanalysis method was0.30%, and the contaminant removed percent at the end of thefirst stage was63.33%, while the contaminant removed percent at the end of the second stage was72.73％. The great performance of the coupling SVE/BV andmicrobial remediation technology that was applied to remove the volatile petroleumhydrocarbons was validated by the field experiments.
Based on the equation of vapor flow of SVE/BV and the analysis of thebiodegradation kinetic model for the contaminated soil with petroleum, the masstransfer model of the coupling SVE/BV and microbial remediation for the treatmentof volatile petroleum hydrocarbons was proposed. Under steady state conditions, thecalculation results of the model of the single component and single extraction wellsystem agreed well with the field data, so the mathematical model that proposed inthis dissertation could be used to provide accurate data for the SVE/BV and microbialremediation treatment of field soil.
The research results of this dissertation, especially the experimental andtheoretical conclusions of the research of the SVE/BV and microbial remediationin-situ treatment of volatile petroleum hydrocarbons, could be used as the basic dataand the reference for the pilot or field treatment of contaminated soil.
引文
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