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NH2-nFe3O4@ZnO@Ce磁性复合材料的制备及其对三氯酚污染物的光催化降解

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赵真艺, 沈鑫怡, 陈定宁, 陈嘉磊, 刘琦, 沈昊宇, 周先波. NH2-nFe3O4@ZnO@Ce磁性复合材料的制备及其对三氯酚污染物的光催化降解[J]. 环境化学, 2020, (3): 643-652. doi: 10.7524/j.issn.0254-6108.2019080501
引用本文: 赵真艺, 沈鑫怡, 陈定宁, 陈嘉磊, 刘琦, 沈昊宇, 周先波. NH2-nFe3O4@ZnO@Ce磁性复合材料的制备及其对三氯酚污染物的光催化降解[J]. 环境化学, 2020, (3): 643-652. doi: 10.7524/j.issn.0254-6108.2019080501
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ZHAO Zhenyi, SHEN Xinyi, CHEN Dingning, CHEN Jialei, LIU Qi, SHEN Haoyu, ZHOU Xianbo. Preparation of NH2-nFe3O4@ZnO@Ce magnetic composite material and its photo-catalytic degradation of 2,4,6-trichlorophenol[J]. Environmental Chemistry, 2020, (3): 643-652. doi: 10.7524/j.issn.0254-6108.2019080501
Citation: ZHAO Zhenyi, SHEN Xinyi, CHEN Dingning, CHEN Jialei, LIU Qi, SHEN Haoyu, ZHOU Xianbo. Preparation of NH2-nFe3O4@ZnO@Ce magnetic composite material and its photo-catalytic degradation of 2,4,6-trichlorophenol[J]. Environmental Chemistry, 2020, (3): 643-652. doi: 10.7524/j.issn.0254-6108.2019080501
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NH2-nFe3O4@ZnO@Ce磁性复合材料的制备及其对三氯酚污染物的光催化降解

  • 1. 浙大宁波理工学院, 生物与化学工程学院, 宁波, 315100;

  • 2. 浙江大学化学化工学院, 杭州, 310027

    • 通讯作者: 沈昊宇, E-mail: hyshen@nit.zju.edu.cn ; 
  • 基金项目:

    国家自然科学基金（51608479，81502421），宁波市自然科学基金（2018A610206），国家级大学生创新创业训练计划项目（201813022009）和浙江省新苗计划项目（2018R401181）资助.

Preparation of NH2-nFe3O4@ZnO@Ce magnetic composite material and its photo-catalytic degradation of 2,4,6-trichlorophenol

  • 1. School of Biological and Chemical Engineering, Zhejiang University Ningbo Institute of Technology, Ningbo, 315100, China;

  • 2. School of Chemical Engineering, Zhejiang University, Hangzhou, 310027, China

    • Corresponding author: SHEN Haoyu, hyshen@nit.zju.edu.cn ; 
  • Fund Project: Supported by the National Natural Science Foundation(51608479,81502421),National Natural Science Foundation of Ningbo(2018A610206),National College Students' Innovation and Entrepreneurship Training Program(201813022009) and Xinmiao Students' Innovation Training Program of Zhejiang Province(2018R401181).

  • 摘要: 采用溶剂热法制备了氨基功能化纳米nFe3O4（NH2-nFe3O4），进一步得到纳米ZnO修饰的NH2-nFe3O4@ZnO和Ce掺杂的磁性复合材料NH2-nFe3O4@ZnO@Ce.通过X-射线衍射（XRD）、傅里叶变换红外光谱（FTIR）、洛伦兹透射电镜（TEM）、扫描电镜（SEM）、振动样品磁强计（VSM）、紫外-可见漫反射（UV-DRS）等手段对其进行了组成、结构、形貌、磁性等表征，并研究了其光催化降解三氯酚（2，4，6-TCP）的性能.系统考察了Ce掺杂量、TCP的初始浓度、溶液pH值等因素对材料的降解性能的影响，初步探讨了降解机理.结果表明，NH2-nFe3O4@ZnO@Ce平均粒径约为50 nm，饱和磁化强度为11.98 emu·g-1.在pH 4.0-7.0，NH2-nFe3O4@ZnO@Ce磁性复合材料可以实现对浓度<20.0 mg·L-1的TCP溶液在60 min内近100%降解.Ce的掺杂和NH2-nFe3O4复合有利于形成掺杂能级、加快光生电子的迁移能力，降低光生电子-空穴对复合率，有效提高材料对TCP的降解性能.NH2-nFe3O4@ZnO@Ce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，是有优异潜力的TCP降解的绿色催化剂.
    Abstract: NH2-nFe3O4 was prepared by solvothermal method. Furtherly, nano-ZnO modified NH2-nFe3O4@ZnO and Ce-doped magnetic composite NH2-nFe3O4@ZnO@Ce were prepared. The magnetic composites were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Lorentz transmission electron microscopy (TEM), scanning electron microscopy (SEM), vibration sample magnetometer (VSM), and diffuse reflectance UV-visible spectroscopy (UV-DRS) etc. Their applications for photocatalytic degradation of trichlorophenol (2,4,6-TCP) were investigated. The effects of Ce doping amount, initial concentration of TCP and solution pH value on the degradation performance were systematically investigated. The degradation mechanism was preliminarily discussed. The results showed that the NH2-nFe3O4@ZnO@Ce had an average size of ~50 nm, with the saturation magnetization intensity of 11.98 emu·g-1. At pH 4.0-7.0, NH2-nFe3O4@ZnO@Ce magnetic composites could degrade nearly 100% of TCP with concentration <20.0 mg·L-1 within 60 minutes. It was favorable to photo-catalytic degradation property of the composite material with Ce doping and NH2-nFe3O4 composition. The formation of doping energy levels and the acceleration of photogenerated electron migration energy were presumed during the photo-catalytic degradation process of 2,4,6-TCP via the NH2-nFe3O4@ZnO@Ce magnetic composite material. After 5 cycles, the degradation rate of TCP could still be maintained above 95%, which implied that the NH2-nFe3O4@ZnO@Ce was a potential green catalyst for TCP degradation.
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  • 收稿日期:  2019-08-05

NH2-nFe3O4@ZnO@Ce磁性复合材料的制备及其对三氯酚污染物的光催化降解

    通讯作者: 沈昊宇, E-mail: hyshen@nit.zju.edu.cn ; 
  • 1. 浙大宁波理工学院, 生物与化学工程学院, 宁波, 315100;
  • 2. 浙江大学化学化工学院, 杭州, 310027
  • 收稿日期:  2019-08-05
基金项目:

国家自然科学基金（51608479，81502421），宁波市自然科学基金（2018A610206），国家级大学生创新创业训练计划项目（201813022009）和浙江省新苗计划项目（2018R401181）资助.

摘要: 采用溶剂热法制备了氨基功能化纳米nFe3O4（NH2-nFe3O4），进一步得到纳米ZnO修饰的NH2-nFe3O4@ZnO和Ce掺杂的磁性复合材料NH2-nFe3O4@ZnO@Ce.通过X-射线衍射（XRD）、傅里叶变换红外光谱（FTIR）、洛伦兹透射电镜（TEM）、扫描电镜（SEM）、振动样品磁强计（VSM）、紫外-可见漫反射（UV-DRS）等手段对其进行了组成、结构、形貌、磁性等表征，并研究了其光催化降解三氯酚（2，4，6-TCP）的性能.系统考察了Ce掺杂量、TCP的初始浓度、溶液pH值等因素对材料的降解性能的影响，初步探讨了降解机理.结果表明，NH2-nFe3O4@ZnO@Ce平均粒径约为50 nm，饱和磁化强度为11.98 emu·g-1.在pH 4.0-7.0，NH2-nFe3O4@ZnO@Ce磁性复合材料可以实现对浓度<20.0 mg·L-1的TCP溶液在60 min内近100%降解.Ce的掺杂和NH2-nFe3O4复合有利于形成掺杂能级、加快光生电子的迁移能力，降低光生电子-空穴对复合率，有效提高材料对TCP的降解性能.NH2-nFe3O4@ZnO@Ce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，是有优异潜力的TCP降解的绿色催化剂.

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