摘要
采用水热法制备了球形四氧化三铁纳米颗粒,对其表面改性后得到两种吸附剂并用于对双酚A的吸附。借助透射电镜、红外光谱分析、热重分析仪和氮气吸脱附等温仪对两种吸附材料进行物理结构表征。结果表明:成功制备了核壳磁性介孔氧化硅纳米吸附剂(Fe_3O_4@mSiO_2),孔径约为2 nm,比表面积约为160 cm~2/g;对其进一步改性得到苯基改性吸附材料(Fe_3O_4@mSiO_2@PhTES)。通过动力学模拟探究了两种吸附剂对双酚A的吸附特性。结果表明:二者对双酚A的吸附动力学均符合拟二级动力学模型,与Fe_3O_4@mSiO_2相比,Fe_3O_4@mSiO_2@PhTES对双酚A的吸附量明显增加,最高达109 mg/g。主要是分子中苯环以π-π共轭方式与吸附剂表面苯基发生作用增强吸附性能。
The spherical Fe_3O_4 nanoparticles were prepared by hydrothermal method.After the surface modification,two adsorbents were obtained and used for the adsorption of bisphenol A.Transmission electron microscopy,infrared spectroscopy,thermogravimetric analyzer and N_2 adsorption and desorption isothermal analyzer were used to characterize the physical structure of the two adsorbents.The results showed that the core-shell magnetic mesoporous silica nano-adsorbent(Fe_3O_4@mSiO_2)was successfully prepared with a pore size of about 2 nm and a specific surface area of about 160 cm~2/g.Further modifications were made to obtain a phenyl-modified adsorbent material(Fe_3O_4@mSiO_2@Ph TES).The adsorption characteristics of two adsorbents on bisphenol A were explored through kinetic.The results showed that the adsorption kinetics of two adsorbents on bisphenol A met the pseudo-second-order kinetic model. Compared with Fe_3O_4@mSiO_2, the adsorption of bisphenol A by Fe_3O_4@mSiO_2@Ph TES increased significantly up to 109 mg/g.It was mainly because the benzene ring in the molecule interacted with the phenyl group on the surface of the adsorbent in a π-π conjugated manner to enhance the adsorption performance.
引文
[1]潘霞霞,李媛媛,黄会静,等.焦化废水中硫氰化物的生物降解及其与苯酚、氨氮的交互影响[J].化工学报,2009,60(12):3089-3096.
[2]Wu X,Yang Y,Wu G,et al.Simulation and optimization of a coking wastewater biological treatment process by activated sludge models(ASM)[J].J.Environ.Manage.,2016,165(45):235-242.
[3]Lee K,Na J,Seo J Y,et al.Magnetic-nanoflocculant-assisted waternonpolar solvent interface sieve for microalgae harvesting[J].ACS Appl.Mater Interfaces,2015,7(33):18336-18343.
[4]李成魁,杜春风,严彪.磁性铁氧化物纳米颗粒的性能与应用进展[J].无机盐工业,2009,41(11):1-4.
[5]LüT,Chen Y,Qi D M,et al.Treatment of emulsified oil wastewaters by using chitosan grafted magnetic nanoparticles[J].Journal of Alloys and Compounds,2017,696(15):1205-1212.
[6]Ma M,Zhang Y,Yu W,et al.Preparation and characterization of magnetite nanoparticles coated by amino silane[J].Colloids and Surfaces A,2003,212(45):219-226.
[7]Zhang Y F,Liu C,Shi Y Y,et al.One-step hydrothermal synthesis of CTAB-modified Si O2for removal of bisphenol A[J].Water Science&Technology,2017,76(4):928-938.
[8]Liu X C,Hu Y,Huang J,et al.Detailed characteristics of adsorption of bisphenol A by highly hydrophobic MCM-41 mesoporous molecular sieves[J].Research on Chemical Intermediates,2016,42(15):7169-7183.
[9]Sun M M,Zhu A M,Zhang Q G,et al.A facile strategy to synthesize monodisperse superparamagnetic OA-modified Fe3O4nanoparticles with PEG assistant[J].Journal of Magnetism and Magnetic Materials,2014,369(58):49-54.
[10]Guo S,Dong S,Wang E.A general route to construct diverse multifunctional Fe3O4-metal hybrid nanostructures[J].Chemistry:A European Jouranal,2009,15(10):2416-2424.
[11]Oleszczuk P,Pan B,Xing B S.Adsorption and desorption of oxytetracycline and carbamazepine by multiwalled carbon nanotubes[J].Environ.Sci.Technol.,2009,43:9167-9173.
[12]Deng Y H,Qi D W,Deng C H,et al.Superparamagnetic high-magnetization microspheres with an Fe3O4@Si O2core and perpendicularly aligned mesoporous Si O2shell for removal of microcystins[J].Journal of the American Chemical Society,2008,130(1):28-29.
[13]White P D,Anthony J.Computational measurement of steric effects the size of organic substituents computed by ligand repulsive energies[J].Organic Chemistry,1999,64(21):7707-7716.
[14]Braunschweig H,Damme A.1-Heteroaromatic-substituted tetraphenylboroles:π-πinteractions between aromatic and antiaromatic rings through a B—C bond[J].Journal of the American Chemical Society,2012,134(49):20169-20177.
[15]Li E Z,Zhang Y B,Du Z P,et al.Bubbles facilitate ODA adsorption and improve flotation recovery at low temperature during KCl flotation[J].Chemical Engineering Research and Design,2017,117:557-563.