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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

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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. doi: 10.7524/j.issn.0254-6108.2017010901
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. doi: 10.7524/j.issn.0254-6108.2017010901
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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. doi: 10.7524/j.issn.0254-6108.2017010901
Citation: 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. doi: 10.7524/j.issn.0254-6108.2017010901
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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

  • 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

  • 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.

Preparation of Fe(Ⅲ)-Salen-functionalized nano-Fe3O4 magnetic composite and its catalytic degradation of 2,4,6-trichlorophenol

  • 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

  • Fund Project: Supported by the National Natural Science Foundation (51608479),National Natural Science Foundation of Zhejiang Province (LY14B04003),National Natural Science Foundation of Ningbo (2014A610092),National College Students' Innovation and Entrepreneurship Training Program (201513022009) and Xinmiao Students' Innovation Training Program of Zhejiang Province (2015R401181).

  • 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-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.
    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.
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  • 收稿日期:  2017-01-09
  • 刊出日期:  2017-08-15

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

  • 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
  • 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.

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-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.

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