超声水热法制备高可见光催化活性的BiOCl-Bi12O17Cl2纳米复合材料去除染料和药物废水

doi:10.1016/S1872-2067(19)63474-1

摘要/Abstract

摘要： 光催化作为一种环境友好型、低能耗的技术，在环境净化等领域倍受关注.传统光催化剂，如TiO₂，ZnO，V₂O₅和WO₃等具有较高的光敏性，其价格低廉，自然无毒，常用于光电反应的应用当中.然而，这些催化剂具有较宽的禁带宽度，只能在紫外光下响应.为此，设计一种较窄带隙的高可见光活性的光催化剂具有一定的意义.近年来，氯氧化铋光催化剂受到了越来越多的关注，其在紫外光下具有非常优异的光催化性能.并且，研究者们已成功合成出非化学计量比的氯氧化铋，如Bi₃O₄Cl（2.60eV），Bi₁₂O₁₇Cl₂（2.10eV），Bi₁₂O₁₅Cl₆（2.86eV）和Bi₂₄O₃₁Cl₁₀（2.70eV）等光催化剂.研究表明，较低的Cl/O比可能会减小催化剂的带隙宽度，并提高其光催化性能；其中Bi₁₂O₁₇Cl₂的Cl/O比最小，是最有潜力的氯氧化铋光催化剂.然而，Bi₁₂O₁₇Cl₂具有较高的光生电子空穴复合率，会极大的减弱其光催化活性.因此，将Bi₁₂O₁₇Cl₂与具有高稳定性，结构相似且空穴复合率低的BiOCl相结合，将会极大提高在可见光下Bi₁₂O₁₇Cl₂的光催化活性.本文采用了超声水热法成功制备了具有高可见光催化活性的BiOCl-Bi₁₂O₁₇Cl₂纳米复合材料，用于去除染料和药物废水.扫描电子显微镜和比表面积分析仪的结果表明，纳米复合材料具有良好的分散性，结构为花瓣形状，其平均厚度为20至50nm，且具有较高的比表面积.紫外-可见漫反射和光致发光光谱分析表明，纳米复合材料具有良好的可见光吸收性能，并且光生电子空穴复合率远低于Bi₁₂O₁₇Cl₂.其在可见光下降解罗丹明B（/环丙沙星）的动力学常数分别约为Bi₁₂O₁₇Cl₂，BiOCl和P25的8.14（/4.94），64.66（/11.91）和42.63（/36.07）倍.合适的形态，结构和光电性能是此纳米复合光催化剂具有优异光催化性能的原因.
此外，该催化剂还显示出较宽的pH适用范围和优异的可重复利用性，有利于实际利用.机理研究表明，降解罗丹明B的主要活性物质是光生空穴和超氧自由基.总之，本文开发了一种绿色、稳定、高效的可见光光催化剂，对BiOCl基的光催化剂的研究作出了一定的贡献.

关键词: BiOCl-Bi₁₂O₁₇Cl₂, 纳米复合材料, 绿色技术, 可见光光催化

Abstract: A BiOCl-Bi₁₂O₁₇Cl₂ nanocomposite with a high visible-light response and a low photoinduced electron-hole pair recombination rate was successfully synthesized using an ultrasonic-hydrothermal method. The texture, structure, optical, and photocatalytic properties of the composite were characterized. The results showed that the composite had a sheet flower-like structure with a large specific surface area. Ultraviolet-visible diffuse reflection spectra and photoluminescence spectra showed that the composite had an excellent visible-light response and a low recombination rate of photoinduced electron hole pairs. The photocatalytic property of the composite was evaluated by the removal efficiency of rhodamine B and ciprofloxacin under visible-light illumination. The composite's reaction rate constant of removing rhodamine B (/ciprofloxacin) was approximately 8.14 (/4.94), 42.63 (/11.91) and 64.66 (/36.07) times that of Bi₁₂O₁₇Cl₂, P25, and BiOCl, respectively. Furthermore, the composite showed a wide applicable pH range and excellent reusability. Mechanism analysis showed that photogenerated holes played a dominant role and ·O₂^- also contributed to photocatalytic degradation. In summary, this study presents a high-efficiency photocatalyst for wastewater treatment.

Key words: BiOCl-Bi₁₂O₁₇Cl₂, Nanocomposite, Green technology, Visible-light photocatalysis

龙泽清, 仙光, 张光明, 张涛, 李雪梅. 超声水热法制备高可见光催化活性的BiOCl-Bi₁₂O₁₇Cl₂纳米复合材料去除染料和药物废水[J]. 催化学报, 2020, 41(3): 464-473.

Zeqing Long, Guang Xian, Guangming Zhang, Tao Zhang, Xuemei Li. BiOCl-Bi₁₂O₁₇Cl₂ nanocomposite with high visible-light photocatalytic activity prepared by an ultrasonic hydrothermal method for removing dye and pharmaceutical[J]. Chinese Journal of Catalysis, 2020, 41(3): 464-473.

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超声水热法制备高可见光催化活性的BiOCl-Bi₁₂O₁₇Cl₂纳米复合材料去除染料和药物废水

BiOCl-Bi₁₂O₁₇Cl₂ nanocomposite with high visible-light photocatalytic activity prepared by an ultrasonic hydrothermal method for removing dye and pharmaceutical

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