Preparation of g-C3N4/FeOCl composite and its photo-Fenton degradation property for RhB under simulate visible light
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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。Abstract: In order to study the photo-Fenton properties of FeOCl combined with carbon materials, g-C3N4/FeOCl nanocomposites were prepared by a simple calcination method according to the different composite mass ratios of g-C3N4 and FeCl3·6H2O. Composition, structure, and optical properties of the composite samples tested by XRD, SEM, TEM, XPS, UV-vis DRS, EIS, and transient photocurrent testing. The results show that the g-C3N4/FeOCl composite has a layered nanorod stacking structure with the good light response and carrier separation capability. When the composite ratio of g-C3N4 to FeCl3·6H2O is 1∶20, it exhibits excellent photo-Fenton performance, and the degradation rate of rhodamine B (RhB) reaches 92.4%. And after three cycles, the efficiency of the composite material in degrading RhB remains at 80.1% that showing good stability. Based on the experimental results, the Z-type heterojunction between g-C3N4 and FeOCl was proposed to improve the separation efficiency of photogenerated carriers, and the possible mechanism of photo-Fenton degradation of RhB by Z-type heterojunction was discussed.
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Key words:
- g-C3N4 /
- FeOCl /
- photo-Fenton activity /
- Z-type heterojunction /
- photoelectrochemical properties
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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 4 FeOCl、g-C3N4和g-C3N4/FeOCl复合材料的UV-vis吸收光谱 (a) 和(αhν)1/2-hν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-hν plotted ((b)-(f))
α—Absorption coefficient; hν—Photon energy; Eg—Energy gap
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 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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