磁性空心纳米反应器及其类芬顿反应催化活性
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摘要
利用二茂铁的水热氧化分解在硅胶颗粒表面包覆Fe_3O_4-C壳层,除去核心硅胶后,制备了一种磁性空心纳米微球。合成的磁性纳米微球直径为280nm,壳层厚度为20nm,为典型的空心结构,其主要成分Fe_3O_4可作为类芬顿反应催化剂,其表面的亲水碳层和空心结构的限域效应进一步增强了催化活性,可高效降解有机污染物,在H_2O_2浓度为1.2mol/L,环境温度为35℃,酸性和中性条件下,0.2g/L的Fe_3O_4-C空心纳米微球在0.5h内能够将1mmol/L的苯酚基本完全降解。而且该纳米反应器具有超顺磁性和较高的饱和磁通量(42.5emu/g),处理之后可以方便地分离回收,以便重复使用,节约了处理成本。
Fe_3O_4-C double shell was fabricated onto the surface of silica sphere template through hydrothermal oxidation decomposition of ferrocene,followed by removal of the silica core to obtain the hollow magnetic microsphere.The magnetic microsphere,with 280 nm in diameter and 20 nm in shell thickness,has typical hollow structure.The major component(Fe_3O_4)could serve as fenton-like catalyst and the superficial hydrophilic carbon layer and the confinement effect of the hollow structure further enhanced the catalytic performance,so that the obtained material exhibited superior degradation ability toward organic pollutant.Thirty min was enough for the nearly complete degradation of 1 mmol/L of phenol under acidic or neutral pH at 35℃(1.2 mol/L of H_2 O_2 and 0.2 g/L of Fe_3O_4-C hollow catalyst).Furthermore,the superparamagnetism and high magnetic saturation value(42.5 emu/g)facilitated the facile recovery of the catalyst from the matrix solution and improved the reusability which greatly saved the treatment cost.
Fe_3O_4-C double shell was fabricated onto the surface of silica sphere template through hydrothermal oxidation decomposition of ferrocene,followed by removal of the silica core to obtain the hollow magnetic microsphere.The magnetic microsphere,with 280 nm in diameter and 20 nm in shell thickness,has typical hollow structure.The major component(Fe_3O_4)could serve as fenton-like catalyst and the superficial hydrophilic carbon layer and the confinement effect of the hollow structure further enhanced the catalytic performance,so that the obtained material exhibited superior degradation ability toward organic pollutant.Thirty min was enough for the nearly complete degradation of 1 mmol/L of phenol under acidic or neutral pH at 35℃(1.2 mol/L of H_2 O_2 and 0.2 g/L of Fe_3O_4-C hollow catalyst).Furthermore,the superparamagnetism and high magnetic saturation value(42.5 emu/g)facilitated the facile recovery of the catalyst from the matrix solution and improved the reusability which greatly saved the treatment cost.
引文
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[3]冯勇,吴德礼,马鲁铭.铁氧化物催化类Fenton反应[J].化学进展,2013,25(7):1219-1228.
[4] YANG M,ZHANG N,XU Y.Synthesis of Fullerene-,Carbon Nanotube-,and Graphene-TiO2Nanocomposite Photocatalysts for Se lective Oxidation:A Comparative Study[J].ACS Appl Mater Inter,2013,5:1156-1164.
[5] LI X,GAI F,GUAN B,et al.Fe@C Core–Shell and Fe@C Yolk–Shell Particles for Effective Removal of 4-Chlorophenol[J].J Mater Chem A,2015,3:3988-3994.
[6] ZHANG S,ZHAO X,NIU H,et al.,Superparamagnetic Fe3O4Nanoparticles as Catalysts for the Catalytic Oxidation of Phenolic and Aniline Compounds[J].J Hazard Mater,2009,167:560-566.
[7] STOBER W,FINK A.Controlled Growth of Monodisperse Silica Spheres in the Micron Size Range[J].J Colloid Interf Sci,1968,26:62-69.
[8] ZENG T,ZHANG X,WANG S,et al.Assembly of a Nanoreactor System with Confined Magnetite Core and Shell for Enhanced Fen ton-Like Catalysis[J].Chem Eur J,2014,20:6474-6481.
[9] HJ503-2009,水质挥发酚的测定4-氨基安替比林分光光度法[S].
[10] WANG T,MA B,JIN A,et al.Facile loading of Ag nanoparticles onto magnetic microsphere by the aid of a tannic acid-metal polymer layer to synthesize magnetic disinfectant with high antibacterial activity[J].J Hazard Mater,2018,342:392-400.
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