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g-C3N4/FeOCl纳米复合材料的制备及其光芬顿降解RhB性能

马金环 魏智强 丁梅杰 赵继威

马金环, 魏智强, 丁梅杰, 等. g-C3N4/FeOCl纳米复合材料的制备及其光芬顿降解RhB性能[J]. 复合材料学报, 2023, 40(10): 5820-5829. doi: 10.13801/j.cnki.fhclxb.20221226.002
引用本文: 马金环, 魏智强, 丁梅杰, 等. g-C3N4/FeOCl纳米复合材料的制备及其光芬顿降解RhB性能[J]. 复合材料学报, 2023, 40(10): 5820-5829. doi: 10.13801/j.cnki.fhclxb.20221226.002
MA Jinhuan, WEI Zhiqiang, DING Meijie, et al. Preparation of g-C3N4/FeOCl composite and its photo-Fenton degradation property for RhB under simulate visible light[J]. Acta Materiae Compositae Sinica, 2023, 40(10): 5820-5829. doi: 10.13801/j.cnki.fhclxb.20221226.002
Citation: MA Jinhuan, WEI Zhiqiang, DING Meijie, et al. Preparation of g-C3N4/FeOCl composite and its photo-Fenton degradation property for RhB under simulate visible light[J]. Acta Materiae Compositae Sinica, 2023, 40(10): 5820-5829. doi: 10.13801/j.cnki.fhclxb.20221226.002

g-C3N4/FeOCl纳米复合材料的制备及其光芬顿降解RhB性能

doi: 10.13801/j.cnki.fhclxb.20221226.002
基金项目: 国家自然科学基金(52268042);甘肃省自然科学基金(22JR5RA253);兰州理工大学红柳一流学科发展项目
详细信息
    通讯作者:

    魏智强,博士,教授,博士生导师,研究方向纳米材料 E-mail: qianweizuo@163.com

  • 中图分类号: TB332

Preparation of g-C3N4/FeOCl composite and its photo-Fenton degradation property for RhB under simulate visible light

Funds: National Natural Science Foundation of China (52268042); Natural Science Foundation of Gansu Province (22JR5RA253); HongLiu First-Class Disciplines Development Program of Lanzhou University of Technology
  • 摘要: 为了研究FeOCl与碳材料复合后的光芬顿性能,采用简单的煅烧法将不同质量比的g-C3N4与FeOCl复合制备出g-C3N4/FeOCl纳米复合材料。通过XRD、SEM、TEM、XPS、UV-vis DRS、EIS和瞬态光电流测试等方法对g-C3N4/FeOCl进行了结构、形貌、元素组成、光电化学性能进行表征。结果表明:g-C3N4/FeOCl复合材料呈层状纳米棒堆叠结构,光响应性能良好,载流子分离能力明显改善。当g-C3N4与FeCl3·6H2O的复合比例为1∶20时表现出优异的光芬顿性能,罗丹明B (RhB)的降解率达到92.4%,并且经过3次循环使用后复合材料降解RhB的效率依然保持在80.1%,表现出良好的稳定性。基于实验结果,提出g-C3N4与FeOCl之间构建成Z型异质结,提高了光生载流子的分离效率,探讨了Z 型异质结光芬顿降解RhB的可能降解机制。

     

  • 图  1  FeOCl、g-C3N4和g-C3N4/FeOCl复合材料的XRD图谱

    Figure  1.  XRD patterns of FeOCl, g-C3N4 and g-C3N4/FeOCl composites

    图  2  (a) FeOCl的SEM图像和粒径分布;g-C3N4/FeOCl-2的TEM (b) 和HRTEM图像 (c)、选区电子衍射 (d)、EDS图 (e) 和TEM-mapping图 ((f)~(l))

    Figure  2.  (a) SEM image and particle size distribution of FeOCl; TEM (b) and HRTEM (c) images, selected area electron diffraction image (d), EDS (e) and TEM-mapping ((f)~(l)) spectra of g-C3N4/FeOCl-2

    d—Interplanar spacing

    图  3  g-C3N4/FeOCl-2和FeOCl的XPS图谱:(a) 全谱;(b) Fe2p;(c) O1s;(d) Cl 2p;(e) C1;(f) N1

    Figure  3.  XPS spectra of the g-C3N4/FeOCl-2 and FeOCl: (a) Survey spectra; (b) Fe2p; (c) O1s; (d) Cl 2p; (e) C1; (f) N1

    图  4  FeOCl、g-C3N4和g-C3N4/FeOCl复合材料的UV-vis吸收光谱 (a) 和(αhν)1/2-曲线估算材料的带隙值 ((b)~(f))

    Figure  4.  UV-vis absorption spectra (a) and the bandgap value of FeOCl, g-C3N4, and g-C3N4/FeOCl composites that estimated by a related curve of (αhν)1/2- plotted ((b)-(f))

    α—Absorption coefficient; —Photon energy; Eg—Energy gap

    图  5  FeOCl、g-C3N4和g-C3N4/FeOCl-2的电化学阻抗谱 (a) 和瞬态光电流谱 (b)

    Figure  5.  Electrochemical impedance spectroscopy (a) and transient photocurrent responses (b) of FeOCl, g-C3N4, and g-C3N4/FeOCl-2 composites

    图  6  FeOCl (a)和g-C3N4 (b)的莫特-肖特基(M-S)图

    Figure  6.  Mott-Schottky (M-S) plots of FeOCl (a) and g-C3N4 (b)

    SCE—Standard calomel electrode

    图  7  FeOCl、g-C3N4和 g-C3N4/FeOCl 降解罗丹明B (RhB)的光芬顿性能 (a) 和相对的一级动力学曲线 (b);g-C3N4/FeOCl-2的循环稳定性 (c) 和自由基捕获试验 (d)

    Figure  7.  Photo-Fenton degradation property (a) and corresponding first-order kinetic curves (b) of FeOCl, g-C3N4 and g-C3N4/FeOCl samples for rhodamine B (RhB); Cycling stability curves (c) and radical-trapping experiment (d) of g-C3N4/FeOCl-2

    Ct—Pollutant concentration at the moment of t; C0—Original pollutant concentration; IPA—Iso-propyl alcohol; p-BQ—p-benzoquinone; IA—Methanol

    图  8  循环实验前(a)和循环实验后(b)的g-C3N4/FeOCl-2的SEM图像

    Figure  8.  SEM images of g-C3N4/FeOCl-2 composites before (a) and after (b) the cycling experiment

    图  9  (a) n-n 型异质结的载流子分布图;(b) g-C3N4/FeOCl-2样品在可见光照射下降解RhB的光芬顿机制

    Figure  9.  (a) Band diagram of n-n type heterojunction; (b) Schematic diagram of photo-Fenton mechanism of g-C3N4/FeOCl-2

    EF—Fermi energy levels; qVD—Built-in electric field; Ed—Energy level difference; NHE—Standard hydrogen electrode; CB—Conduction band; VB—Valence band

    表  1  g-C3N4/FeOCl复合材料的命名

    Table  1.   Naming of g-C3N4/FeOCl composites

    Sample Mass ratio g-C3N4∶FeCl3·6H2O
    g-C3N4/FeOCl-1 1∶15
    g-C3N4/FeOCl-2 1∶20
    g-C3N4/FeOCl-3 1∶25
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  • 收稿日期:  2022-10-24
  • 修回日期:  2022-12-08
  • 录用日期:  2022-12-10
  • 网络出版日期:  2022-12-26
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