(壳聚糖/γ-Fe_2O_3)@C磁性复合材料表面印迹聚合物选择性吸附2,4,5-TCP的研究
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摘要
本文采用乳液聚合法合成碳基磁性碳球(壳聚糖/γ-Fe2O3)@C,并在其表面上引入乙烯基,以2,4,5-三氯酚(2,4,5-TCP)为模板分子、甲基丙烯酸(MAA)为功能单体、乙二醇二甲基丙烯酸酯(EGDMA)为交联剂制备磁性碳球表面印迹聚合物。并利用扫描电子显微镜、紫外分光光度计、振动样品磁强计和热重分析仪等表征手段对其形貌、结构等物理化学性能进行表征,研究其热稳定性和磁稳定性,考察其作为吸附剂对2,4,5-三氯酚的吸附性能及选择性能。研究结果表明,磁性碳球和磁性碳球表面印迹聚合物(MMIPs)的饱和磁强度分别为4.3 emu/g和1.7 emu/g。吸附平衡数据表明其符合Freundlich吸附等温模型,平衡吸附量大约为200mg/g,吸附符合准二级动力学方程,平衡吸附时间大约为10 min,印迹吸附剂对模板分子吸附量最佳,且存在明显特异性吸附。
A carbon-based magnetic carbon sphere of(chitosan/maghemite)@C was synthesized by emulsion polymerization,and vinyl groups were introduced into its surface.The imprinted polymer on the magnetic carbon sphere surface was prepared using 2,4,5-trichlorophenol(TCP) as a template molecule,methacrylic acid(MAA) as a functional monomer,and ethylene glycol dimethylacrylate(EGDMA) as the cross-linker.The morphology,structure,and other physicochemical properties of the formed material were characterized by means of a scanning electron microscope(SEM),ultraviolet(UV) spectrophotometer,vibration sample magnetometer(VSM),and thermogravimetric analyzer(TGA).Thermostability and magnetic stability of the material were studied,and the adsorption performance and selectivity of the material as an adsorbent for 2,4,5-TCP were investigated.The results indicated that saturation magnetization values of the magnetic carbon sphere and magnetic carbon sphere surface imprinted polymers(MMIPs) were 4.3 and 1.7 emu/g,respectively.The equilibrium adsorption data conformed to the Freundlich isotherm model,equilibrium adsorption capacity was ~200 mg/g,and the kinetics followed a second-order kinetic equation.The adsorption equilibrium time was approximately ten minutes,and the imprinted sorbent showed optimal adsorption on the template molecule,with significant specific adsorption.
A carbon-based magnetic carbon sphere of(chitosan/maghemite)@C was synthesized by emulsion polymerization,and vinyl groups were introduced into its surface.The imprinted polymer on the magnetic carbon sphere surface was prepared using 2,4,5-trichlorophenol(TCP) as a template molecule,methacrylic acid(MAA) as a functional monomer,and ethylene glycol dimethylacrylate(EGDMA) as the cross-linker.The morphology,structure,and other physicochemical properties of the formed material were characterized by means of a scanning electron microscope(SEM),ultraviolet(UV) spectrophotometer,vibration sample magnetometer(VSM),and thermogravimetric analyzer(TGA).Thermostability and magnetic stability of the material were studied,and the adsorption performance and selectivity of the material as an adsorbent for 2,4,5-TCP were investigated.The results indicated that saturation magnetization values of the magnetic carbon sphere and magnetic carbon sphere surface imprinted polymers(MMIPs) were 4.3 and 1.7 emu/g,respectively.The equilibrium adsorption data conformed to the Freundlich isotherm model,equilibrium adsorption capacity was ~200 mg/g,and the kinetics followed a second-order kinetic equation.The adsorption equilibrium time was approximately ten minutes,and the imprinted sorbent showed optimal adsorption on the template molecule,with significant specific adsorption.
引文
[1]Field A J,Sierra-Alvarez R.Microbial degradation of chlorinated phenols[J].Rev.Environ.Sci.Biotechnol.,2008,7(3):211-241
[2]M Dilaver,F Kargi.2,4-Dichlorophenol(DCP)containing wastewater treatment using a hybrid-loop bioreactor[J].Biores.Tech.,2009,100(3):1459-1462
[3]S G Poulopoulos,M Nikolaki,D Karampetsos,et al.Photochemical treatment of 2-chlorophenol aqueous solutions using ultraviolet radiation,hydrogen peroxide and photo-fenton reaction[J].J.Hazard.Mater.,2008,153(1-2):582-587
[4]B H Hameed.Equilibrium and kinetics studies of2,4,6-trichlorophenol adsorption onto activated clay[J].Colloids Surf.A.,2007,307(1-3):45-52
[5]Wenjing Zhu,Wei Ma,Chunxiang Li,et al.Magnetic molecularly imprinted microspheres via yeast stabilized Pickering emulsion polymerization for selective recognition of-cyhalothrin[J].Colloids and Surfaces A:Physicochem.Eng.Aspects,2014,453:27-36
[6]Li-juan An,Jing Wang,Zhi-yuan Pang,et al.Magnetic molecularly imprinted silica gel for enrofloxacin recognition[J].Colloids and Surfaces A:Physicochem.Eng.Aspects,2014,452(1):125-128
[7]Leceta I,Guerrero P,de la Caba K.Functional properties of chitosan based films[J].Carbohydrate Polymers,2013,93(1):339-346
[8]Pan J M,Zou X H,Wang X,et al.Selective recognition of2,4-dichlorophenol from aqueous solution by uniformly sized molecularly imprinted microspheres withβ-cyclodextrin/attapulgite composites as support[J].Chemical Engineering Journal,2010,162(3):910-918
[9]Grant T M,King C J.Mechanism of irreversible adsorption of phenolic compounds by activated carbons[J].Industrial&Engineering Chemistry Research,1990,29(2):264-271
[10]Fernyhough C,Ryan A J,Battaglia G.p H controlled assembly of a polybutadiene-poly(methacrylic acid)copolymer in water:packing considerations and kinetic limitations[J].Soft Matter,2009,5(8):1674-1682
[11]Allen S J,Mckay G,Porter J F.Adsorption isotherm models for basic dye adsorption by peat in single and binary component systems[J].Journal of Colloid and Interface Science,2004,280(2):322-333
[12]Mazzotti M.Equilibrium theory based design of simulated moving bed processes for a generalized Langmuir isotherm[J].Journal of Chromatography A,2006,1126(1):311-322
[13]Ho Y S,Mc Kay G.The sorption of lead(Ⅱ)ions on peat[J].Water Research,1999,33(2):578-584
[14]Ho Y S,Mc Kay G.Pseudo-second order model for sorption processes[J].Process Biochemistry,1999,34(5):451-465
[15]Wu Z J,Joo H,Lee K.Kinetics and thermodynamics of the organic dye adsorption on the mesoporous hybrid xeroge[J].Chemical Engineering Journal,2005,112(1):227-236
[2]M Dilaver,F Kargi.2,4-Dichlorophenol(DCP)containing wastewater treatment using a hybrid-loop bioreactor[J].Biores.Tech.,2009,100(3):1459-1462
[3]S G Poulopoulos,M Nikolaki,D Karampetsos,et al.Photochemical treatment of 2-chlorophenol aqueous solutions using ultraviolet radiation,hydrogen peroxide and photo-fenton reaction[J].J.Hazard.Mater.,2008,153(1-2):582-587
[4]B H Hameed.Equilibrium and kinetics studies of2,4,6-trichlorophenol adsorption onto activated clay[J].Colloids Surf.A.,2007,307(1-3):45-52
[5]Wenjing Zhu,Wei Ma,Chunxiang Li,et al.Magnetic molecularly imprinted microspheres via yeast stabilized Pickering emulsion polymerization for selective recognition of-cyhalothrin[J].Colloids and Surfaces A:Physicochem.Eng.Aspects,2014,453:27-36
[6]Li-juan An,Jing Wang,Zhi-yuan Pang,et al.Magnetic molecularly imprinted silica gel for enrofloxacin recognition[J].Colloids and Surfaces A:Physicochem.Eng.Aspects,2014,452(1):125-128
[7]Leceta I,Guerrero P,de la Caba K.Functional properties of chitosan based films[J].Carbohydrate Polymers,2013,93(1):339-346
[8]Pan J M,Zou X H,Wang X,et al.Selective recognition of2,4-dichlorophenol from aqueous solution by uniformly sized molecularly imprinted microspheres withβ-cyclodextrin/attapulgite composites as support[J].Chemical Engineering Journal,2010,162(3):910-918
[9]Grant T M,King C J.Mechanism of irreversible adsorption of phenolic compounds by activated carbons[J].Industrial&Engineering Chemistry Research,1990,29(2):264-271
[10]Fernyhough C,Ryan A J,Battaglia G.p H controlled assembly of a polybutadiene-poly(methacrylic acid)copolymer in water:packing considerations and kinetic limitations[J].Soft Matter,2009,5(8):1674-1682
[11]Allen S J,Mckay G,Porter J F.Adsorption isotherm models for basic dye adsorption by peat in single and binary component systems[J].Journal of Colloid and Interface Science,2004,280(2):322-333
[12]Mazzotti M.Equilibrium theory based design of simulated moving bed processes for a generalized Langmuir isotherm[J].Journal of Chromatography A,2006,1126(1):311-322
[13]Ho Y S,Mc Kay G.The sorption of lead(Ⅱ)ions on peat[J].Water Research,1999,33(2):578-584
[14]Ho Y S,Mc Kay G.Pseudo-second order model for sorption processes[J].Process Biochemistry,1999,34(5):451-465
[15]Wu Z J,Joo H,Lee K.Kinetics and thermodynamics of the organic dye adsorption on the mesoporous hybrid xeroge[J].Chemical Engineering Journal,2005,112(1):227-236