引用本文:
蒋琦, 姜哲昊, 陈荣, 郭素芳, 冯锦秀, 沈昊宇, 胡美琴, 夏清华. Fe(Ⅲ)-Salen功能化纳米Fe3O4复合材料的合成及其对三氯苯的催化降解性能[J]. 环境化学, 2017, 36(8): 1744-1751
JIANG Qi, JIANG Zhehao, CHEN Rong, GUO Sufang, FENG Jinxiu, SHEN Haoyu, HU Meiqin, XIA Qinghua. Preparation of Fe(Ⅲ)-Salen-functionalized nano-Fe3O4 magnetic composite and its catalytic degradation of 2,4,6-trichlorophenol[J]. Environmental Chemistry, 2017, 36(8): 1744-1751

Fe(Ⅲ)-Salen功能化纳米Fe3O4复合材料的合成及其对三氯苯的催化降解性能
蒋琦1, 姜哲昊1, 陈荣1, 郭素芳1, 冯锦秀1, 沈昊宇1, 胡美琴1, 夏清华2
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
摘要:
采用溶剂热制备了氨基功能化纳米Fe3O4 磁性复合材料(NH2-nFe3O4), 并进一步通过缩合、配位等反应得到Fe(Ⅲ)-Salen功能化纳米Fe3O4复合材料(nFe3O4@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, nFe3O4@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nFe3O4@Fe(Ⅲ)Salen, 研究了其在可见光/H2O2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nFe3O4@Fe(Ⅲ)Salen用量 ≥ 0.8 g·L-1,溶液pH值为4.0-7.0, H2O2浓度为 8.16-40.8 mmol·L-1时, nFe3O4@Fe(Ⅲ)Salen/H2O2/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, nFe3O4@Fe(Ⅲ)Salen是有优异潜力的水中TCP绿色催化剂.
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   
Preparation of Fe(Ⅲ)-Salen-functionalized nano-Fe3O4 magnetic composite and its catalytic degradation of 2,4,6-trichlorophenol
JIANG Qi1, JIANG Zhehao1, CHEN Rong1, GUO Sufang1, FENG Jinxiu1, SHEN Haoyu1, HU Meiqin1, XIA Qinghua2
1. Ningbo Institute of Technology, Zhejiang University, Ningbo, 315100, China;
2. Ministry-of-Education Key Laboratory for the Synthesis and Applications of Organic Functional Molecules, Hubei Collaborative Innovation Center for Advanced Organochemical Materials, Hubei University, Wuhan, 430062, China
Abstract:
Amino-functionalized nano-Fe3O4 magnetic particle (NH2-nFe3O4) was prepared by solvothermal method. Fe(Ⅲ)-Salen nano-Fe3O4 magnetic composite material (nFe3O4@Fe(Ⅲ)Salen) was synthesized by condensation and coordination reactions. The nFe3O4@Fe(Ⅲ)Salen was characterized 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 nFe3O4@Fe(Ⅲ)Salen was around 200 nm, with the saturation magnetization intensity of 24.8 emu·g-1. The nFe3O4@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 nFe3O4@Fe(Ⅲ)Salen dosage was above 0.8 g·L-1, the solution pH value was between 4.0-7.0, and H2O2 concentration between 8.16-40.8 mmol·L-1, the degradation rate of 2,4,6-TCP with initial concentrations of less than 50.0 mg·L-1 (253.2 mg·L-1) reached nearly 100% under the nFe3O4@Fe(Ⅲ)Salen/H2O2/vis system within 5 min, which spanned a wider pH range than the regular Fenton system. nFe3O4@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.
Key words:    Fe(Ⅲ)-Salen functional nano-Fe3O4    magnetic composite material    2,4,6-trichlorophenol    degradation    Fenton-like reaction   
收稿日期: 2017-01-09
基金项目: 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)和浙江省新苗计划项目(2015R401181)资助.
沈昊宇,Tel:0574-88130130,E-mail:hyshen@nit.zju.edu.cn
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