Preparation of g-C3N4/FeOCl composite and its photo-Fenton degradation property for RhB under Simulate visible light
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摘要:
目的 近年来，随着社会的快速发展，越来越多的国家开始注意环境问题，尤其是水环境的污染问题。水资源短缺和人类生产生活需水量的增加使得污水净化处理这一话题变热。 方法 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例的g-CN与FeOCl复合制备出g-CN/FeOCl纳米复合材料。通过X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、紫外-可见光漫反射光谱(UV-vis DRS)、电化学阻抗测试(EIS)和瞬态光电流测试等方法对g-CN/FeOCl进行了成分、结构和光学性质表征。 结果 结果表明：g-CN/FeOCl复合材料呈层状纳米棒堆叠结构，光响应性能良好。当g-CN与FeOCl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%。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。 结论 (1)选用煅烧法在250℃和550℃下制备了FeOCl和g-CN，在FeOCl基上引入无金属聚合物g-CN二者形成Z型异质结材料。XRD、TEM、XPS和EDS表明FeOCl与g-CN复合成功。(2)紫外可见漫反射光谱表明g-CN/FeOCl复合材料的带隙宽度介于FeOCl与g-CN之间，具有更好的可见光吸收性能。(3)电化学测试表明g-CN/FeOCl复合材料具有优异的光生载流子的迁移和分离能力。(4)光芬顿降解RhB测试中，g-CN/FeOCl-2的一阶动力学反应速率常数是纯的FeOCl的1.94倍。(5)通过活性物种捕获实验和能带结构的分析，得出g-CN/FeOCl在降解过程中以Z型异质结的载流子迁移路径进行。 Abstract: In order to study the photo-Fenton properties of FeOCl combined with carbon materials, g-C3N4/FeOCl nanocomposites are 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, 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 FeOCl 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 remained 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.-
Key words:
- g-C3N4 /
- FeOCl /
- photo-Fenton activity /
- Z-type heterojunction /
- Photoelectrochemical properties
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图 1 FeOCl、g-C3N4和g-C3N4/FeOCl复合材料的XRD图谱
Figure 1. XRD patterns of pure FeOCl, pure g-C3N4, and g-C3N4/FeOCl composites
图 2 FeOCl的SEM图和内插图为纳米棒粒径图(a)，g-C3N4/FeOCl-2的TEM(b)和HRTEM图(c)、选区电子衍射(d)、EDS图(e)和TEM-mapping图(f~k)
Figure 2. (a) SEM and Particle size images of FeOCl; (b) TEM and (c) HRTEM; (d) Selected Area Electron Diffraction images and (e) EDS and (f~k) TEM-Mapping spectra of g-C3N4/FeOCl-2
图 3 g-C3N4/FeOCl-2和FeOCl的：(a)XPS全谱,(b)Fe 2 p、(c)O 1 s、(d)Cl 2 p，(e)C 1 s和(f)N 1 s的分谱
Figure 3. (a) XPS survey spectra and (b) also XPS spectra of Fe 2 p, (c) O 1 s, (d) Cl 2 p, (e) C 1 s, and (f) N 1 s in the g- C3N4/FeOCl-2
图 4 FeOCl、g-C3N4和g-C3N4/FeOCl复合材料的：(a)UV-vis吸收光谱和(b-f)(αhν)1/2-hν曲线
Figure 4. (a) UV-vis absorption spectra and (b-f) the (αhν)1/2 - hν curve of pure FeOCl, pure g-C3N4, and g-C3N4/FeOCl composite
图 5 FeOCl、g-C3N4和g-C3N4/FeOCl-2的：(a)电化学阻抗谱和(b)瞬态光电流谱
Figure 5. (a) Electrochemical impedance spectroscopy and (b) Transient photocurrent responses of pure FeOCl, g-C3N4, and g-C3N4/FeOCl-2 samples
图 7 FeOCl、g-C3N4和 g-C3N4/FeOCl 降解RhB的光芬顿性能(a)和相对的一阶动力学曲线(b)，g-C3N4/FeOCl-2的循环稳定性图(c)和自由基捕获图(d)
Figure 7. (a) Photo-Fenton degradation property of FeOCl, g-C3N4 and g-C3N4/FeOCl samples for RhB, (b) Corresponding first-order kinetic curve, (c) Cycling stability curve, and (d) Radical-trapping experiment of g-C3N4/FeOCl-2
Ct−Pollutant concentration at the moment of t; C0−Original pollutant concentration
图 8 g-C3N4/FeOCl-2的SEM图(a)循环实验前和(b)循环实验后
Figure 8. Images of g-C3N4/FeOCl-2 material (a) before and (b) after the cycling experiment
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