黄河兰州段底泥对硝基苯的吸附行为
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摘要
选择硝基苯为代表性污染物,研究了黄河兰州段底泥对硝基苯的动力学吸附和热力学吸附过程,并对离子強度、pH值和粒径等对吸附的影响进行了分析.结果表明,硝基苯在黄河兰州段底泥上的动力学吸附经历了3个阶段:快速、慢速和吸附平衡阶段,0~2h为快速吸附阶段,2~15h为慢吸附阶段,15h后吸附达到平衡.黄河兰州段底泥对硝基苯的动力学吸附过程较好地符合准二级吸附动力学模型;热力学吸附较好地符合Langmuir等温吸附模型;在吸附过程中,吸附自由能△G~θ小于0,焓变△H~θ及熵变△,S~θ均大于0,表明黄河兰州段底泥对硝基苯的吸附是ー个自发吸热且吸附体系的混乱度増大的等温吸附过程.吸附影响因素分析结果显示:当Ca~(2+)离子浓度在0~0.05mol/L时,黄河兰州段底泥对硝基苯的吸附量随Ca~(2+)离子浓度的増大而增加,当Ca~(2+)离子浓度増大到0.1mol/L时,吸附量減少,说明在此离子强度下,Ca~(2+)抑制了底泥对硝基苯的吸附.当pH3~5和7~10范围内时,底泥对硝基苯的吸附量随pH值增大明显减小,当pH5~7范围内时,吸附量随pH值增大基本保持不变.底泥粒径对黄河兰州段底泥吸附硝基苯有显著影响,其饱和吸附量随底泥粒径的减小而增大.
The primary objective of this study was to investigate the adsorption kinetics and thermodynamics of nitrobenzene onto sediment in Lanzhou section of the Yellow River.Meanwhile,the effective factors,such as ionic strength,pH values and the different particle sizes of sediment,were also conducted to characterize the adsorption process.The results showed that the adsorption of nitrobenzene onto sediment in Lanzhou section of the Yellow River has experienced three processes:high-speed adsorption process,deceleration and adsorption equilibrium process.The adsorption equilibrium was reached within 15 h.The adsorption of nitrobenzene onto sediment in Lanzhou of the Yellow River could be better described by the pseudo-second-order kinetic model;the adsorption thermodynamics of nitrobenzene onto sediment is fitted well with the Langmuir isothermal model.Thermodynamics parameters such as the change of free energy,enthalpy and entropy were also evaluated for the adsorption of nitrobenzene onto sediment.The results indicate a spontaneous endothermic and an increase of the chaos in adsorption process.Analysis results of adsorption showed when the concentration of Ca~(2+) was in a range of 0~0.05mol/L,adsorption of nitrobenzene onto sediment increased with the increase of Ca~(2+) concentration,however,when the concentration of Ca~(2+) increased from 0.05 to 0.lmol/L,the adsorption capacity decreased,because the presence of Ca~(2+) inhibited the adsorption of nitrobenzene onto sediment.The pH values and the different particle sizes of sediment have obvious effect on adsorption of nitrobenzene onto sediment.When the pH was in a range of 3~5 and 7~10,the adsorption capacity of nitrobenzene on sediments significantly decreased with the increase of pH,while pH was in a range of 5~7,the adsorption capacity remained unchanged with the increase of pH.The particle size of sediment in Lanzhou section of the Yellow River has significant effect on the adsorption capacity of nitrobenzene,which increase with decrease of the particle size of the sediment.
The primary objective of this study was to investigate the adsorption kinetics and thermodynamics of nitrobenzene onto sediment in Lanzhou section of the Yellow River.Meanwhile,the effective factors,such as ionic strength,pH values and the different particle sizes of sediment,were also conducted to characterize the adsorption process.The results showed that the adsorption of nitrobenzene onto sediment in Lanzhou section of the Yellow River has experienced three processes:high-speed adsorption process,deceleration and adsorption equilibrium process.The adsorption equilibrium was reached within 15 h.The adsorption of nitrobenzene onto sediment in Lanzhou of the Yellow River could be better described by the pseudo-second-order kinetic model;the adsorption thermodynamics of nitrobenzene onto sediment is fitted well with the Langmuir isothermal model.Thermodynamics parameters such as the change of free energy,enthalpy and entropy were also evaluated for the adsorption of nitrobenzene onto sediment.The results indicate a spontaneous endothermic and an increase of the chaos in adsorption process.Analysis results of adsorption showed when the concentration of Ca~(2+) was in a range of 0~0.05mol/L,adsorption of nitrobenzene onto sediment increased with the increase of Ca~(2+) concentration,however,when the concentration of Ca~(2+) increased from 0.05 to 0.lmol/L,the adsorption capacity decreased,because the presence of Ca~(2+) inhibited the adsorption of nitrobenzene onto sediment.The pH values and the different particle sizes of sediment have obvious effect on adsorption of nitrobenzene onto sediment.When the pH was in a range of 3~5 and 7~10,the adsorption capacity of nitrobenzene on sediments significantly decreased with the increase of pH,while pH was in a range of 5~7,the adsorption capacity remained unchanged with the increase of pH.The particle size of sediment in Lanzhou section of the Yellow River has significant effect on the adsorption capacity of nitrobenzene,which increase with decrease of the particle size of the sediment.
引文
谢丹平,李开明,江栋,等.底泥修复对城市污染河道水体污染修复的影响研究[J].环境工程学报,2009,3(8):1447-1453.
许炼烽,邓绍龙,陈继鑫,等.河流底泥污染及其控制与修复[J].生态环境学报,2014,23(10):1708-1715.
李俊生,徐靖,罗建武,等.硝基苯环境效应的研究综述[J].生态环境学报,2009,18(1):368-373.
Qin Q D,Ma J,Liu K.adsorption of nitrobenzene from aqueous solution by MCM-41[J].Journal of Colloid Interface Science,2007,315(1):80-86.
魏世强.环境化学[M].北京:中国农业出版社,2006.
邱立萍,王文科.双氧水-高锰酸钾催化氧化降解地下水中硝基苯的效能与机理[J].环境工程学报,2011,5(4):735-740.
郑佳佳,王睿睿,林志浩,等.壬基酚、五氯酚及硝基苯对端足类河蜾蠃蜚(Corophium acherusicum)的毒性效应[J].生态毒理学报,2014,9(6):1104-1111.
王莹,穆景利,王菊英.我国硝基苯的海水水质基准及生态风险评估研究[J].生态毒理学报,2015,10(1):160-168.
Chen J,Tian S H,Kong L J,et al.Efficient degradation of nitrobenzene by an integrated heterogeneous catalytic ozonation and membrane separation system with active Mg O(111)catalyst[J].Desalination and Water Treatment,2015,56(8):2168-2180.
王亮亮,王志良,王彧,等.吸附树脂负载铁酞菁催化降解硝基苯的研究[J].环境科技,2011,24(6):1-3.
谢刚,毛宁,周林成,等.改进碳纳米管/聚氨酯复合材料吸附硝基苯[J].环境工程学报,2015,9(3):1117-1123.
李媛媛,陈桐,杨丹,等.纳米氧化硅/活性炭复合材料的制备及吸附性能研究[J].化工新型材料,2015,43(2):138-140.
黎先发.木质素活性炭的制备及其对硝基苯的吸附[J].化工环保,2014,34(4):305-310.
陈爱辉,梁慧星,丁成.硝基苯在米草湿地土壤中的吸附特征[J].土壤通报,2013,44(5):1123-1128.
宋艳宇,宋长春,柴俊海,等.湿地土壤对硝基苯的吸附-解吸作用[J].环境科学学报,2009,29(1):140-145.
荆肇乾,彭英艳,胡静.杨树叶改性吸附剂对硝基苯的吸附性能研究[J].科学技术与工程,2015,15(24):140-143.
张继义,李金涛,鲁华涛,等.小麦秸秆生物碳质吸附剂从水中吸附硝基苯的机理[J].环境科学研究,2012,25(3):333-339.
罗雪梅,刘昌明.离子强度对土壤与沉积物吸附多环芳烃的影响研究[J].生态环境,2006,15(5):983-987.
詹树娇,田森林,龙坚,等.阳离子型可逆表面活性剂在膨润土上的吸附行为[J].中国环境科学,2014,34(7):1831-1837.
黎冰,解启来,廖天,等.扎龙湿地表层沉积物有机氯农药的污染特征及风险评价[J].农业环境科学学报,2013,32(2):347-353.
Fatih D.Potential use of shell biomass(Juglans regia L.)for dye removal:Relationships between kinetic pseudo-second-order model parameters and biosorption efficiency[J].Desalination and Water Treatment,2014,5(1-3):219-226.
Munir K,Yusuf M,Noreen Z,et al.Isotherm studies for determination of removal capacity of bi-metal(Ni and Cr)ions by Aspergil lusniger[J].Pakistam Journal of Botany,2010,42(1):593-604.
蒋煜峰,Uwamungu Jean Yves,孙航,等.添加小麦秸秆生物炭对黄土吸附苯甲腈的影响[J].中国环境科学,2016,36(5):1506-1513.
Zaghouane-Boudiaf H,Boutahala M,Tiar C,et al.Treatment of 2,4,5-trichlorophenol by Mg Al-SDBS organo-layered double hydroxides:kinetic and equilibrium studies[J].Chemical Engineering Journal,2011,173(1):36-41.
Chang M Y,Juang R S.Adsorption of tannic acid,humic acid,and dyes from water using the composite of chitosan and activated clay[J].Journal of Colloid and Interface Science,2004,278(1):18-25.
李建炜.活性炭对废水中对氯硝基苯吸附特性研究[C]//中国环境科学学会学术年会论文集,2010,3:3062-3065.
杨成建,曾清如,张静,等.非离子表面活性剂在土壤/沉积物中的吸附模型研究[J].农业环境科学学报,2007,26(4):1396-1401.
马百文,赵勇胜,孙威,等.非水相硝基苯在含水层中的迁移释放规律[J].环境工程学报,2010,4(7):1463-1467.
Kiran I,Akar T,Ozcan A S,et al.Biosorption kinetics and isotherm of Acid Red 57by dried Cephalosporium aphidicola cells from aqueous solution[J].Biochemical Engineering Journal,2006,31:197-203.
康露,吴景贵,张晋京,等.土壤及土壤矿物对类胡敏酸的吸附解吸及其影响因素研究[J].环境科学学报,2013,33(5):1332-1340.
林建伟,詹艳慧,陆霞.锆改性沸石对水中磷酸盐和铵的吸附特性[J].中国环境科学,2012,32(11):2023-2031.
Filius J D,Lumsdon D G,Meeussen J C L,et al.Adsorption of fulvic acid on geothite[J].Geochimica Et Cosmochimica Acta,2000,64(1):51-60.
Vermhlen K,Lewandowski H,Narres H D,et al.Adsorption of polyelectrolytes onto oxides-the influence of ionic strength,molar mass,and Ca2+ions[J].Colloids and Surfaces APhysicochemical and Engineering Aspects,2000,163(1):45-53.
Al-Degs Y S,El-Barghouthi M I,El-Sheikh A H,et al.Effect of solution p H,ionic strength,and temperature on adsorption behavior of reactive dyes on activated carbon[J].Dyes Pigments,2008,77:16-23.
Sennerfors T,Solberg D,Tiberg F.Adsorption of polyelectrolyte-nanoparticle syetems on silica:influence of ionic strength[J].Journal of Colloid and Interface Science,2002,254(2):222-226.
梁锐杰,陈炳稔.流动注射分光光度法研究离子强度对活性炭吸附阴离子染料的影响[J].离子交换与吸附,2004,20(1):54-61.
何江,关伟,李桂海,等.几种酚类化合物在黄河水体沉积物上吸附行为的实验研究[J].农业环境科学学报,2005,24(3):480-485.
张莹.苯酚在典型矿物和沉积物上的吸附降解行为研究[D].沈阳:辽宁大学,2012,15-18.
汤烜祎.改性泥炭吸附水体中疏水性有机污染物及其机理研究[D].上海:华东理工大学,2010.
许炼烽,邓绍龙,陈继鑫,等.河流底泥污染及其控制与修复[J].生态环境学报,2014,23(10):1708-1715.
李俊生,徐靖,罗建武,等.硝基苯环境效应的研究综述[J].生态环境学报,2009,18(1):368-373.
Qin Q D,Ma J,Liu K.adsorption of nitrobenzene from aqueous solution by MCM-41[J].Journal of Colloid Interface Science,2007,315(1):80-86.
魏世强.环境化学[M].北京:中国农业出版社,2006.
邱立萍,王文科.双氧水-高锰酸钾催化氧化降解地下水中硝基苯的效能与机理[J].环境工程学报,2011,5(4):735-740.
郑佳佳,王睿睿,林志浩,等.壬基酚、五氯酚及硝基苯对端足类河蜾蠃蜚(Corophium acherusicum)的毒性效应[J].生态毒理学报,2014,9(6):1104-1111.
王莹,穆景利,王菊英.我国硝基苯的海水水质基准及生态风险评估研究[J].生态毒理学报,2015,10(1):160-168.
Chen J,Tian S H,Kong L J,et al.Efficient degradation of nitrobenzene by an integrated heterogeneous catalytic ozonation and membrane separation system with active Mg O(111)catalyst[J].Desalination and Water Treatment,2015,56(8):2168-2180.
王亮亮,王志良,王彧,等.吸附树脂负载铁酞菁催化降解硝基苯的研究[J].环境科技,2011,24(6):1-3.
谢刚,毛宁,周林成,等.改进碳纳米管/聚氨酯复合材料吸附硝基苯[J].环境工程学报,2015,9(3):1117-1123.
李媛媛,陈桐,杨丹,等.纳米氧化硅/活性炭复合材料的制备及吸附性能研究[J].化工新型材料,2015,43(2):138-140.
黎先发.木质素活性炭的制备及其对硝基苯的吸附[J].化工环保,2014,34(4):305-310.
陈爱辉,梁慧星,丁成.硝基苯在米草湿地土壤中的吸附特征[J].土壤通报,2013,44(5):1123-1128.
宋艳宇,宋长春,柴俊海,等.湿地土壤对硝基苯的吸附-解吸作用[J].环境科学学报,2009,29(1):140-145.
荆肇乾,彭英艳,胡静.杨树叶改性吸附剂对硝基苯的吸附性能研究[J].科学技术与工程,2015,15(24):140-143.
张继义,李金涛,鲁华涛,等.小麦秸秆生物碳质吸附剂从水中吸附硝基苯的机理[J].环境科学研究,2012,25(3):333-339.
罗雪梅,刘昌明.离子强度对土壤与沉积物吸附多环芳烃的影响研究[J].生态环境,2006,15(5):983-987.
詹树娇,田森林,龙坚,等.阳离子型可逆表面活性剂在膨润土上的吸附行为[J].中国环境科学,2014,34(7):1831-1837.
黎冰,解启来,廖天,等.扎龙湿地表层沉积物有机氯农药的污染特征及风险评价[J].农业环境科学学报,2013,32(2):347-353.
Fatih D.Potential use of shell biomass(Juglans regia L.)for dye removal:Relationships between kinetic pseudo-second-order model parameters and biosorption efficiency[J].Desalination and Water Treatment,2014,5(1-3):219-226.
Munir K,Yusuf M,Noreen Z,et al.Isotherm studies for determination of removal capacity of bi-metal(Ni and Cr)ions by Aspergil lusniger[J].Pakistam Journal of Botany,2010,42(1):593-604.
蒋煜峰,Uwamungu Jean Yves,孙航,等.添加小麦秸秆生物炭对黄土吸附苯甲腈的影响[J].中国环境科学,2016,36(5):1506-1513.
Zaghouane-Boudiaf H,Boutahala M,Tiar C,et al.Treatment of 2,4,5-trichlorophenol by Mg Al-SDBS organo-layered double hydroxides:kinetic and equilibrium studies[J].Chemical Engineering Journal,2011,173(1):36-41.
Chang M Y,Juang R S.Adsorption of tannic acid,humic acid,and dyes from water using the composite of chitosan and activated clay[J].Journal of Colloid and Interface Science,2004,278(1):18-25.
李建炜.活性炭对废水中对氯硝基苯吸附特性研究[C]//中国环境科学学会学术年会论文集,2010,3:3062-3065.
杨成建,曾清如,张静,等.非离子表面活性剂在土壤/沉积物中的吸附模型研究[J].农业环境科学学报,2007,26(4):1396-1401.
马百文,赵勇胜,孙威,等.非水相硝基苯在含水层中的迁移释放规律[J].环境工程学报,2010,4(7):1463-1467.
Kiran I,Akar T,Ozcan A S,et al.Biosorption kinetics and isotherm of Acid Red 57by dried Cephalosporium aphidicola cells from aqueous solution[J].Biochemical Engineering Journal,2006,31:197-203.
康露,吴景贵,张晋京,等.土壤及土壤矿物对类胡敏酸的吸附解吸及其影响因素研究[J].环境科学学报,2013,33(5):1332-1340.
林建伟,詹艳慧,陆霞.锆改性沸石对水中磷酸盐和铵的吸附特性[J].中国环境科学,2012,32(11):2023-2031.
Filius J D,Lumsdon D G,Meeussen J C L,et al.Adsorption of fulvic acid on geothite[J].Geochimica Et Cosmochimica Acta,2000,64(1):51-60.
Vermhlen K,Lewandowski H,Narres H D,et al.Adsorption of polyelectrolytes onto oxides-the influence of ionic strength,molar mass,and Ca2+ions[J].Colloids and Surfaces APhysicochemical and Engineering Aspects,2000,163(1):45-53.
Al-Degs Y S,El-Barghouthi M I,El-Sheikh A H,et al.Effect of solution p H,ionic strength,and temperature on adsorption behavior of reactive dyes on activated carbon[J].Dyes Pigments,2008,77:16-23.
Sennerfors T,Solberg D,Tiberg F.Adsorption of polyelectrolyte-nanoparticle syetems on silica:influence of ionic strength[J].Journal of Colloid and Interface Science,2002,254(2):222-226.
梁锐杰,陈炳稔.流动注射分光光度法研究离子强度对活性炭吸附阴离子染料的影响[J].离子交换与吸附,2004,20(1):54-61.
何江,关伟,李桂海,等.几种酚类化合物在黄河水体沉积物上吸附行为的实验研究[J].农业环境科学学报,2005,24(3):480-485.
张莹.苯酚在典型矿物和沉积物上的吸附降解行为研究[D].沈阳:辽宁大学,2012,15-18.
汤烜祎.改性泥炭吸附水体中疏水性有机污染物及其机理研究[D].上海:华东理工大学,2010.