Fe(Ⅲ)-Salen功能化纳米Fe_3O_4复合材料的合成及其对三氯苯的催化降解性能  

Preparation of Fe( Ⅲ)-Salen-functionalized nano-Fe_3O_4 magnetic composite and its catalytic degradation of 2,4,6-trichlorophenol

作　　者：蒋琦[1] 姜哲昊[1] 陈荣[1] 郭素芳[1] 冯锦秀 沈昊宇[1] 胡美琴[1] 夏清华[2] 

机构地区：[1]浙江大学宁波理工学院,生物与化学工程学院,宁波315100 [2]湖北大学,有机化工新材料湖北省协同创新中心,有机功能分子合成与应用教育部重点实验室,武汉430062

出　　处：《环境化学》2017年第8期1744-1751,共8页Environmental Chemistry

基　　金：国家自然科学基金(51608479);浙江省自然科学基金(LY14B04003);宁波市自然科学基金(2014A610092);国家级大学生创新创业训练计划项目(201513022009);浙江省新苗计划项目(2015R401181)资助~~

摘　　要：采用溶剂热制备了氨基功能化纳米Fe_3O_4磁性复合材料(NH2-nFe_3O_4),并进一步通过缩合、配位等反应得到Fe(Ⅲ)-Salen功能化纳米Fe_3O_4复合材料(nFe_3O_4@Fe(Ⅲ)Salen).通过元素分析(EA)、X-射线衍射(XRD)、红外光谱(FTIR)、透射电镜(TEM)、振动样品磁强计(VSM)等手段对其进行了组成、结构、形貌、磁性等表征.结果表明,nFe_3O_4@Fe(Ⅲ)Salen平均粒径为约200 nm,饱和磁化强度为24.8 emu·g-1.催化剂为nFe_3O_4@Fe(Ⅲ)Salen,研究了其在可见光/H_2O_2类Fenton体系催化降解水中2,4,6-三氯酚(2,4,6-TCP)的性能.研究发现,当nFe_3O_4@Fe(Ⅲ)Salen用量≥0.8 g·L^(-1),溶液pH值为4.0—7.0,H_2O_2浓度为8.16—40.8 mmol·L^(-1)时,nFe_3O_4@Fe(Ⅲ)Salen/H_2O_2/可见光体系可以实现对浓度<50.0 mg·L^(-1)(253.2 mg·L^(-1))的TCP溶液在5 min内近100%降解,较普通Fenton反应体系有更宽的pH适用范围.循环使用5次后,该催化体系对TCP的降解率仍能保持95%以上,nFe_3O_4@Fe(Ⅲ)Salen是有优异潜力的水中TCP绿色催化剂.Amino-functionalized nano-Fe_3O_4 magnetic particle（ NH2-n Fe_3O_4） was prepared by solvothermal method. Fe（ Ⅲ）-Salen nano-Fe_3O_4 magnetic composite material（ n Fe_3O_4@ Fe（ Ⅲ）Salen） was synthesized by condensation and coordination reactions. The n Fe_3O_4@ Fe（ Ⅲ） Salen wascharacterized by elementary analysis, powder X-ray diffraction, Fourier-transformed infrared spectroscopy,transmission electron microscopy and vibrating sample magnetometer. The results show that the average particle size of n Fe_3O_4@ Fe（ Ⅲ） Salen was around 200 nm,with the saturation magnetization intensity of 24.8 emu·g-1. The n Fe_3O_4@ Fe（ Ⅲ） Salen was used as a heterogeneous catalyst for the degradation of 2,4,6-TCP via Fenton-like reaction under visible light. The results showed that when n Fe_3O_4@ Fe（ Ⅲ） Salen dosage was above 0.8 g·L^（-1）,the solution pH value was between 4.0—7.0,and H_2O_2 concentration between 8.16—40.8 mmol·L^（-1）,the degradation rate of2,4,6-TCP with initial concentrations of less than 50. 0 mg·L^（-1）（ 253.2 mg·L^（-1）） reached nearly100% under the n Fe_3O_4@ Fe（ Ⅲ） Salen/H_2O_2/vis system within 5 min,which spanned a wider pH range than the regular Fenton system. n Fe_3O_4@ Fe（ Ⅲ） Salen was reused after recycling for 5 times,with the degradation rate of 2,4,6-TCP still over 95%. It is a potentialy effective and reusable material for the catalytic degradation of 2,4,6-TCP.

关 键 词：Fe(Ⅲ)-Salen功能化纳米Fe3O4 磁性复合材料 2 4 6-三氯酚 降解 类FENTON反应 

分 类 号：O643.36[理学—物理化学] X703[理学—化学]