磁性金属有机骨架Fe_3O_4@ZIF-8的制备及对偶氮染料刚果红的高效吸附
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摘要
采用常温搅拌法,在聚苯乙烯磺酸钠(PSS)处理过的Fe_3O_4表面诱导生长ZIF-8壳层,成功合成了磁性核壳金属有机骨架Fe_3O_4@ZIF-8,并对其吸附去除偶氮染料刚果红的性能进行了探究,考察了刚果红初始浓度和接触时间、Fe_3O_4@ZIF-8投加量以及pH对刚果红去除的影响。SEM、TEM、XRD、FT-IR及VSM表征结果证明,ZIF-8纳米颗粒已成功负载于Fe_3O_4表面,形成了典型的核壳结构,并且具有优异的磁学性能。吸附实验结果表明,反应最佳pH为6,吸附剂投加量为500 mg·L~(-1);当反应时间达到180 min时,吸附达到平衡。吸附反应的吸附动力学和吸附等温线分析表明,刚果红染料在Fe_3O_4@ZIF-8上的吸附动力学符合二级动力学方程,吸附等温线符合Langmuir模型。Fe_3O_4@ZIF-8吸附剂对刚果红具有高效的选择吸附性能并且在循环吸附中展现出良好的循环吸附性能。因此,磁性核壳金属有机骨架Fe_3O_4@ZIF-8作为吸附剂在去除刚果红染料方面有着广阔的应用前景。
The magnetic core-shell metal organic framework Fe_3O_4@ZIF-8 was successfully synthesized by treating the surface of Fe_3O_4 with sodium polystyrene sulfonate(PSS) and inducing ZIF-8 shell growth on it under continuous stirring at room temperature. The performance of adsorption and removal of azo dye congo red by Fe_3O_4@ZIF-8 was investigated. The effects of initial concentration and contact time, Fe_3O_4@ZIF-8 dosage and pH on congo red removal were investigated. The characterization of SEM, TEM, XRD, FT-IR and VSM showed that ZIF-8 nanoparticles have been successfully loaded on the surface of Fe_3O_4 to form a typical coreshell structure with excellent magnetic properties. The experimental results showed that the optimum pH was 6,the dosage of adsorbent was 500 mg·L~(-1), and the adsorption equilibrium was achieved at the reaction time of180 min. The adsorption kinetics of congo red on Fe_3O_4@ZIF-8 was in accordance with the second-order kinetic equation, and the adsorption isotherm followed Langmuir model. Fe_3O_4@ZIF-8 adsorbent had high selective adsorption performance for congo red and presented good reusability in cyclic adsorption. Therefore, magnetic core-shell metal-organic framework Fe_3O_4@ZIF-8 had broad application prospects in the removal of congo red dyes as adsorbent.
The magnetic core-shell metal organic framework Fe_3O_4@ZIF-8 was successfully synthesized by treating the surface of Fe_3O_4 with sodium polystyrene sulfonate(PSS) and inducing ZIF-8 shell growth on it under continuous stirring at room temperature. The performance of adsorption and removal of azo dye congo red by Fe_3O_4@ZIF-8 was investigated. The effects of initial concentration and contact time, Fe_3O_4@ZIF-8 dosage and pH on congo red removal were investigated. The characterization of SEM, TEM, XRD, FT-IR and VSM showed that ZIF-8 nanoparticles have been successfully loaded on the surface of Fe_3O_4 to form a typical coreshell structure with excellent magnetic properties. The experimental results showed that the optimum pH was 6,the dosage of adsorbent was 500 mg·L~(-1), and the adsorption equilibrium was achieved at the reaction time of180 min. The adsorption kinetics of congo red on Fe_3O_4@ZIF-8 was in accordance with the second-order kinetic equation, and the adsorption isotherm followed Langmuir model. Fe_3O_4@ZIF-8 adsorbent had high selective adsorption performance for congo red and presented good reusability in cyclic adsorption. Therefore, magnetic core-shell metal-organic framework Fe_3O_4@ZIF-8 had broad application prospects in the removal of congo red dyes as adsorbent.
引文
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[21]张湛杭,张景丽,刘建明.金属有机骨架ZIF-67对刚果红的吸附性研究[J].天津城建大学学报,2017,23(4):267-272.
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[3]GREENWALD M J,REDDING A M,CANNON F S.A rapid kinetic dye test to predict the adsorption of 2-methylisoborneol onto granular activated carbons and to identify the influence of pore volume distributions[J].Water Research,2015,68:784-792.
[4]LIU F,GUO Z,LING H,et al.Effect of pore structure on the adsorption of aqueous dyes to ordered mesoporous carbons[J].Microporous&Mesoporous Materials,2016,227:104-111.
[5]YANG R,LI H J,HUANG M,et al.A review on chitosan-based flocculants and their applications in water treatment[J].Water Research,2016,95:59-89.
[6]CHAMPNESS N R,SCHRODER M.Extended networks formed by coordination polymers in the solid state[J].Current Opinion in Solid State&Materials Science,1998,3(4):419-424.
[7]LU W G,WEI Z W,GU Z Y,et al.Tuning the structure and function of metal-organic frameworks via linker design[J].Chemical Society Reviews,2014,43(16):5561-5593.
[8]EVANS J D,SUMBY C J,DOONAN C J.Post-synthetic metalation of metal-organic frameworks[J].Chemical Society Reviews,2014,43(16):5933-5951.
[9]LEE J Y,FARHA O K,ROBERTS J,et al.Metal-organic framework materials as catalysts[J].Chemical Society Reviews,2009,38(5):1450-1459.
[10]KRENO L E,KIRSTY L,FARHA O K,et al.Metal-organic framework materials as chemical sensors[J].Chemical Reviews,2011,112(2):1105-1125.
[11]LI J R,JULIAN S,ZHOU H C.Metal-organic frameworks for separations[J].Chemical Reviews,2012,112(2):869-932.
[12]张琪颖.基于金属有机骨架材料的高效吸附剂研发[D].济南:济南大学,2016.
[13]孙杨,陆广明,唐祝兴.磁性纳米材料Fe3O4@MOF-5的制备及其对刚果红吸附性能的研究[J].辽宁化工,2017,46(11):12-14.
[14]张通.ZIF-8包覆的核-壳结构材料的合成及其应用[D].大连:大连理工大学,2015.
[15]ZHOU L C,MENG X G,FU J W,et al.Highly efficient adsorption of chlorophenols onto chemically modified chitosan[J].Applied Surface Science,2014,292(1):735-741.
[16]MOGHADDAM H K,PAKIZEH M.Experimental study on mercury ions removal from aqueous solution by MnO2/CNTs nanocomposite adsorbent[J].Journal of Industrial&Engineering Chemistry,2015,21:221-229.
[17]LORENC-GRABOWSKA E,RUTKOWSKI P.High basicity adsorbents from solid residue of cellulose and synthetic polymer co-pyrolysis for phenol removal:Kinetics and mechanism[J].Applied Surface Science,2014,316(1):435-442.
[18]YANG G,CHEN H L,QIN H D,et al.Amination of activated carbon for enhancing phenol adsorption:Effect of nitrogencontaining functional groups[J].Applied Surface Science,2014,293(3):299-305.
[19]LI B J,CAO H Q,SHAO J,et al.Superparamagnetic Fe3O4 nanocrystals@graphene composites for energy storage devices[J].Journal of Materials Chemistry,2011,21(13):5069-5075.
[20]顾兵.沸石咪唑酯骨架结构材料(ZIF-8)对染料废水中刚果红的吸附效果和特征分析研究[D].南京:南京农业大学,2015.
[21]张湛杭,张景丽,刘建明.金属有机骨架ZIF-67对刚果红的吸附性研究[J].天津城建大学学报,2017,23(4):267-272.
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