微乳液法用于落地原油应急处理及资源回收的研究
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摘要
以十二烷基苯磺酸钠(SDBS)为表面活性剂配制微乳液对落地原油污染土壤进行应急处理及回收原油模拟实验。将原始与回收的原油、土壤进行对比发现:回收土壤的pH略高且大致呈中性,Zeta电位更小,黏粒体积分数减小,微乳液处理对土壤的理化性质影响较小;回收原油中饱和分含量升高,芳香分、胶质和沥青质含量降低,密度与黏度都降低,表明回收所得的是轻质原油。分析了SDBS、正丁醇、NaCl添加量及油水比对原油脱除率的影响,并对筛选出的3种配方微乳液进行温度、循环利用和放大实验检验原油脱除效果的稳定性,最终确定w(SDBS)=10%、w(n-butanol)=4.8%、w(NaCl)=0.8%、w(diesel)=12.8%的微乳液为处理落地原油的最优配方。
Sodium dodecyl benzene sulfonate(SDBS) was used as a surfactant to prepare microemulsion for emergency treatment of crude oil contaminated soil and recovery of crude oil. Comparison between the original and the recovered crude oil and soil samples was done. It is found that the pH of the recovered soil is slightly higher, the Zeta potential is smaller, the volume fraction of clay reduced, indicating that the microemulsion treatment has little influence on the physical and chemical properties of the soil. The recovered crude oil has higher saturation fraction,lower aromatic, resin and asphaltene content, lower density and viscosity, and belongs to light crude oil. The effects of SDBS, n-butanol and NaCl contents on de-oiling effect were investigated. Experiments on effects of oil/water ratio, temperature, recycling and scaling-up were carried out by using the selected three types of microemulsions formula. The optimal microemulsion formula for the de-oiling of crude oil contaminated soil is w(SDBS)=10%, w(nbutanol)=4.8%, w(NaCl)=0.8%, w(diesel)=12.8%.
Sodium dodecyl benzene sulfonate(SDBS) was used as a surfactant to prepare microemulsion for emergency treatment of crude oil contaminated soil and recovery of crude oil. Comparison between the original and the recovered crude oil and soil samples was done. It is found that the pH of the recovered soil is slightly higher, the Zeta potential is smaller, the volume fraction of clay reduced, indicating that the microemulsion treatment has little influence on the physical and chemical properties of the soil. The recovered crude oil has higher saturation fraction,lower aromatic, resin and asphaltene content, lower density and viscosity, and belongs to light crude oil. The effects of SDBS, n-butanol and NaCl contents on de-oiling effect were investigated. Experiments on effects of oil/water ratio, temperature, recycling and scaling-up were carried out by using the selected three types of microemulsions formula. The optimal microemulsion formula for the de-oiling of crude oil contaminated soil is w(SDBS)=10%, w(nbutanol)=4.8%, w(NaCl)=0.8%, w(diesel)=12.8%.
引文
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[17]张强,汪晓东,金日光.油酸/氨水-醇-汽油-水微乳体系拟三元相图的分析[J].北京化工大学学报(自然科学版),2001,28(2):37-39.Zhang Q,Wang X D,Jin R G.Analysis on the phase diagrams of pseudo-tricomponent of oleic acid/ammonia-gasoline-alcoholwater microemulsion system[J].Journal of Beijing University of Chemical Technology(Natural Science Edition),2001,28(2):37-39.
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[19]董松祥.微乳化清洁柴油的配制及其性能研究[D].青岛:中国石油大学,2010.Dong S X.Study on the preparation and performance of energysaving and clean micro-emulsified diesel oil[D].Qingdao:China University of Petroleum,2010.
[20]曹建喜,罗立文,董松祥,等.微乳柴油的研制及性能[J].中国石油大学学报(自然科学版),2010,34(4):152-156.Cao J X,Luo L W,Dong S X,et al.Preparation and properties of micro-emulsified diesel[J].Journal of China University of Petroleum(Edition of Natural Science),2010,34(4):152-156.
[21]Mcclements D J.Nanoemulsions versus microemulsions:terminology,differences,and similarities[J].Soft Matter,2012,8(6):1719-1729.
[22]Jeirani Z,Jan B M,Ali B S,et al.Formulation,optimization and application of triglyceride microemulsion in enhanced oil recovery[J].Industrial Crops and Products,2013,43(1):6-14.
[23]Bellocq A M.Effects of alcohol chain length and salt on phase behavior and critical phenomena in SDS microemulsions[M]//Kumar P,Mittal K L.Handbook of Microemulsion Science and Technology.New York:Marcel Dekker,Inc.,1999:139-184.
[24]Pei G,Zhu Y,Cai X,et al.Surfactant flushing remediation of odichlorobenzene and p-dichlorobenzene contaminated soil[J].Chemosphere,2017,185:1112-1121.
[25]Qiao B W,Ye S,Wu J,et al.Surfactant‐enhanced electroosmotic flushing in a trichlorobenzene contaminated clayey soil[J].Ground Water,2018,56(4):673-679.
[26]Guan Z,Tang X Y,Nishimura T,et al.Surfactant-enhanced flushing enhances colloid transport and alters macroporosity in diesel-contaminated soil[J].Journal of Environmental Sciences,2018,64(2):197-206.
[27]Hernandez H W,Ehlert W,Trabelsi S.Removal of crude oil residue from solid surfaces using microemulsions[J].Fuel,2019,237:398-404.
[28]Lowry E,Sedghi M,Goual L.Molecular simulations of NAPLremoval from mineral surfaces using microemulsions and surfactants[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2016,506:485-494.
[29]Daoshan L I,Demin W,Wanli K.Interfacial viscoelasticity of water/decan containing resins and asphatenes[J].Journal of Chemical Industry&Engineering,2003,54(8):1164-1168.
[30]Liu H E,Zhou P P,Wu Z H,et al.Solubilization behavior of organic mixtures in optimum Winsor typeⅢmicroemulsion systems of sodium dodecyl sulfate[J].Journal of Surfactants and Detergents,2018,2(14):497-507.
[31]Liu H E,Wu Z H,Jing J G,et al,Partition of n-butanol among phases and solubilization ability of Winsor typeⅢmicroemulsions[J].Journal of Surfactants and Detergents,2016,19:713-724.
[32]靖建歌,刘会娥,丁传芹,等.内标法研究WinsorⅢ型微乳液的醇分布及其增溶参数[J].化学工程,2015,43(1):32-36.Jing J G,Liu H E,Ding C Q,et al.Alcohol distribution and solubilization parameters of WinsorⅢmicroemulsion using internal standard method[J].Chemical Engineering(China),2015,43(1):32-36.
[33]Javanbakht G,Goual L.Mobilization and micellar solubilization of NAPL contaminants in aquifer rocks[J].Journal of Contaminant Hydrology,2016,185/186:61-73.
[2]赵红艳,韩毅,吕娟,等.三种洗涤剂淋洗落地原油污染土壤的试验研究[J].东北师大学报(自然科学版),2009,41(1):123-126.Zhao H Y,Han Y,Lyu J,et al.Test on three kinds of detergent washing the soils contaminated by crude oil[J].Journal of Northeast Normal University(Natural Science Edition),2009,41(1):123-126.
[3]廉景燕,哈莹,黄磊,等.石油污染土壤物化修复前后生物毒性效应[J].环境科学,2011,32(3):870-874.Lian J Y,Ha Y,Huang L,et al.Biological toxicity effect of petroleum contaminated soil before and after physicochemical remediation[J].Environmental Science,2011,32(3):870-874.
[4]吴蔓莉,张晨,祁燕云,等.生物修复对黄土壤中石油烃的去除作用及影响因素[J].农业环境科学学报,2018,37(6):1159-1165.Wu M L,Zhang C,Qi Y Y,et al.Degradation of petroleum hydrocarbons during the bioremediation of cultivated loessial soil[J].Journal of Agro Environment Science,2018,37(6):1159-1165.
[5]Salager J L,Forgiarini A M,Bullón J.How to attain ultralow interfacial tension and three-phase behavior with surfactant formulation for enhanced oil recovery:a review(1):Optimum formulation for simple surfactant-oil-water ternary systems[J].Journal of Surfactants and Detergents,2013,16(4):449-472.
[6]李佳,曹兴涛,隋红,等.石油污染土壤修复技术研究现状与展望[J].石油学报(石油加工),2017,33(5):811-833.Li J,Cao X T,Sui H,et al.Overview of remediation technologies for petroleum-contaminated soils[J].Acta Petrolei Sinica(Petroleum Processing Section),2017,33(5):811-833.
[7]Kellay H,Binks B P,Hendrikx Y,et al.Properties of surfactant monolayers in relation to microemulsion phase behaviour[J].Advances in Colloid&Interface Science,2017,49:85-112.
[8]Salager J L,Antón R E,Sabatini D A,et al.Enhancing solubilization in microemulsions state of the art and current trends[J].Journal of Surfactants and Detergents,2005,8(1):3-21.
[9]Koneva A S,Safonova E A,Kondrakhina P S,et al.Effect of water content on structural and phase behavior of water-in-oil(ndecane)microemulsion system stabilized by mixed nonionic surfactants Span 80/Tween 80[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2017,518:273-282.
[10]Salager J L,Forgiarini A M,Márquez L,et al.How to attain an ultralow interfacial tension and three-phase behavior with surfactant formulation for enhanced oil recovery:a review(2):Performance improvement trends from Winsor.s premise to currently proposed inter-and intra-molecular mixtures[J].Journal of Surfactants and Detergents,2013,16(5):631-663.
[11]Santanna V C,Curbelo F D S,Castro Dantas T N,et al.Microemulsion flooding for enhanced oil recovery[J].Journal of Petroleum Science and Engineering,2009,66(3/4):117-120.
[12]Ogino K,Abe M.Microemulsion formation with some typical surfactants[J].Surface and Colloid Science,1993,15:85-123.
[13]Bera A,Mandal A.Microemulsions:a novel approach to enhanced oil recovery:a review[J].Journal of Petroleum Exploration and Production Technology,2015,5(3):255-268.
[14]夏雪,刘会娥,丁传芹,等.酸碱性对十二烷基硫酸钠-正丁醇-煤油-水微乳液体系的影响[J].石油化工,2011,40(10):1110-1114.Xia X,Liu H E,Ding C Q,et al.Influence of acidity and alkalinity on sodium dodecyl sulfate-n-butanol-kerosene-water microemulsion system[J].Petrochemical Technology,2011,40(10):1110-1114.
[15]夏雪,刘会娥,夏晔,等.SDS/正丁醇/煤油/水微乳液体系的相转变研究[J].高校化学工程学报,2011,25(6):911-915.Xia X,Liu H E,Xia Y,et al.Phase inversion of sodium dodecyl sulfate(SDS)/n-butanol/kerosene/water microemulsion system[J].J.Chem.Eng.Chinese Univ.,2011,25(6):911-915.
[16]张孝坤,刘会娥,丁传芹,等.不同电解质对SDS/正丁醇/煤油/水微乳液体系的影响[J].高校化学工程学报,2013,27(6):1089-1093.Zhang X K,Liu H E,Ding C Q,et al.Influence of different types of electrolyte on sodium dodecyl sulfate/butanol/kerosene/water microemulsion system[J].J.Chem.Eng.Chinese Univ.,2013,27(6):1089-1093.
[17]张强,汪晓东,金日光.油酸/氨水-醇-汽油-水微乳体系拟三元相图的分析[J].北京化工大学学报(自然科学版),2001,28(2):37-39.Zhang Q,Wang X D,Jin R G.Analysis on the phase diagrams of pseudo-tricomponent of oleic acid/ammonia-gasoline-alcoholwater microemulsion system[J].Journal of Beijing University of Chemical Technology(Natural Science Edition),2001,28(2):37-39.
[18]周雅文,张高勇,王红霞.汽油微乳化技术研究[J].日用化学工业,2002,,32(2):1-4.Zhou Y W,Zhang G Y,Wang H X.Study on the technology of water-in-gasoline microemulsion[J].China Surfactant Detergent&Cosmetics,2002,32(2):1-4.
[19]董松祥.微乳化清洁柴油的配制及其性能研究[D].青岛:中国石油大学,2010.Dong S X.Study on the preparation and performance of energysaving and clean micro-emulsified diesel oil[D].Qingdao:China University of Petroleum,2010.
[20]曹建喜,罗立文,董松祥,等.微乳柴油的研制及性能[J].中国石油大学学报(自然科学版),2010,34(4):152-156.Cao J X,Luo L W,Dong S X,et al.Preparation and properties of micro-emulsified diesel[J].Journal of China University of Petroleum(Edition of Natural Science),2010,34(4):152-156.
[21]Mcclements D J.Nanoemulsions versus microemulsions:terminology,differences,and similarities[J].Soft Matter,2012,8(6):1719-1729.
[22]Jeirani Z,Jan B M,Ali B S,et al.Formulation,optimization and application of triglyceride microemulsion in enhanced oil recovery[J].Industrial Crops and Products,2013,43(1):6-14.
[23]Bellocq A M.Effects of alcohol chain length and salt on phase behavior and critical phenomena in SDS microemulsions[M]//Kumar P,Mittal K L.Handbook of Microemulsion Science and Technology.New York:Marcel Dekker,Inc.,1999:139-184.
[24]Pei G,Zhu Y,Cai X,et al.Surfactant flushing remediation of odichlorobenzene and p-dichlorobenzene contaminated soil[J].Chemosphere,2017,185:1112-1121.
[25]Qiao B W,Ye S,Wu J,et al.Surfactant‐enhanced electroosmotic flushing in a trichlorobenzene contaminated clayey soil[J].Ground Water,2018,56(4):673-679.
[26]Guan Z,Tang X Y,Nishimura T,et al.Surfactant-enhanced flushing enhances colloid transport and alters macroporosity in diesel-contaminated soil[J].Journal of Environmental Sciences,2018,64(2):197-206.
[27]Hernandez H W,Ehlert W,Trabelsi S.Removal of crude oil residue from solid surfaces using microemulsions[J].Fuel,2019,237:398-404.
[28]Lowry E,Sedghi M,Goual L.Molecular simulations of NAPLremoval from mineral surfaces using microemulsions and surfactants[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2016,506:485-494.
[29]Daoshan L I,Demin W,Wanli K.Interfacial viscoelasticity of water/decan containing resins and asphatenes[J].Journal of Chemical Industry&Engineering,2003,54(8):1164-1168.
[30]Liu H E,Zhou P P,Wu Z H,et al.Solubilization behavior of organic mixtures in optimum Winsor typeⅢmicroemulsion systems of sodium dodecyl sulfate[J].Journal of Surfactants and Detergents,2018,2(14):497-507.
[31]Liu H E,Wu Z H,Jing J G,et al,Partition of n-butanol among phases and solubilization ability of Winsor typeⅢmicroemulsions[J].Journal of Surfactants and Detergents,2016,19:713-724.
[32]靖建歌,刘会娥,丁传芹,等.内标法研究WinsorⅢ型微乳液的醇分布及其增溶参数[J].化学工程,2015,43(1):32-36.Jing J G,Liu H E,Ding C Q,et al.Alcohol distribution and solubilization parameters of WinsorⅢmicroemulsion using internal standard method[J].Chemical Engineering(China),2015,43(1):32-36.
[33]Javanbakht G,Goual L.Mobilization and micellar solubilization of NAPL contaminants in aquifer rocks[J].Journal of Contaminant Hydrology,2016,185/186:61-73.
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