ZnCuAl-LDH/Bi2MoO6纳米复合材料的构建及其可见光催化降解性能

doi:10.3866/PKU.WHXB201911016

摘要/Abstract

摘要：

本工作采用稳态共沉淀法制备了ZnCuAl-LDH/Bi₂MoO₆ (LDH/Bi₂MoO₆)纳米复合材料，并研究了所得材料在可见光下降解污染物罗丹明B (RhB)的光催化性能。结果表明，所得LDH/Bi₂MoO₆纳米复合材料比单纯的ZnCuAl-LDH和Bi₂MoO₆具有显著提高的光催化活性和较好的稳定性。光催化性能的提高得益于异质结的形成以及高的比表面积，从而有利于光生电子-空穴对的有效分离和更多光催化活性位点的暴露。研究发现，在光降解过程中，所产生的•OH和O₂^•−是主要的反应性物种，而e⁻和h⁺的贡献较少。基于实验结果，提出了一种可能的光催化机制。本工作提供了一种制备基于LDH和(或)Bi₂MoO₆纳米复合材料的方法，所得LDH/Bi₂MoO₆纳米复合材料可望作为一种可见光光催化剂，在净化环境和缓解资源短缺方面有潜在应用。

关键词: 层状双氢氧化物, Bi₂MoO₆, 纳米复合材料, 活性位点, 可见光降解, 异质结

Abstract:

In this study, pure Bi₂MoO₆ was synthesized via a solvothermal method. A ZnCuAl-layered double hydroxide (LDH)/Bi₂MoO₆ (denoted as LDH/Bi₂MoO₆) nanocomposite was synthesized via a steady-state co-precipitation route using Bi₂MoO₆ as the matric material. LDH was deposited on the surface of Bi₂MoO₆ with a close contact interface. The specific surface area of the resulting LDH/Bi₂MoO₆ composite increased up to 19.1 m²∙g⁻¹ owing to the stacking arrangement between LDH and the Bi₂MoO₆ nanosheets, resulting in the generation of a large number of reactive sites. In addition, the light absorption region of the LDH/Bi₂MoO₆ composite was larger than those of pure LDH and Bi₂MoO₆ because of the formation of a heterojunction structure and the possible quantum size effect. The photocatalytic performance of the as-prepared samples was evaluated by carrying out the degradation of rhodamine B (RhB) using them under visible light irradiation. Compared to pure LDH and Bi₂MoO₆, the LDH/Bi₂MoO₆ nanocomposite exhibited enhanced photocatalytic activity for the degradation of RhB. With an increase in the LDH content, the photocatalytic activity of the LDH/Bi₂MoO₆ composite first increased and then decreased. Although the addition of an optimum amount of LDH was beneficial for the generation of electron-hole pairs, excessive LDH on the surface of Bi₂MoO₆ decreased the visible light absorption ability of both the components, thus reducing photocatalytic activity of the composite. This indicates that an appropriate LDH:Bi₂MoO₆ molar ratio is necessary for obtaining LDH/Bi₂MoO₆ composites with excellent photocatalytic activity. Furthermore, the LDH/Bi₂MoO₆ composite showed high photocatalytic stability and reusability. The structure of the LDH/Bi₂MoO₆ composite remained almost unchanged even after four photodegradation cycles. The enhanced photocatalytic performance of the composite can be attributed to the combined effect of its heterojunction structure and high specific surface area, which are beneficial for effective separation of photogenerated charge carriers and the availability of a large number of active sites for photocatalysis. It was found that •OH and O₂^•− were the main reactive species, while e⁻ and h⁺ contributed little to the photodegradation process. The generation, transfer, and separation of photoinduced electrons and holes in the composites were investigated by transient photocurrent responses, electrochemical impedance spectroscopy Nyquist plots, and photoluminescence measurements. The results showed that the heterojunction structure of the composites played a key role in enhancing their photocatalytic activity. A possible photodegradation mechanism was proposed for the composite. This study will provide a facile approach for the preparation of LDH- and/or Bi₂MoO₆-based nanocomposites. The LDH/Bi₂MoO₆ nanocomposite prepared in this study showed huge potential to be used as a visible-light photocatalyst for degrading environmental pollutants.

Key words: Layered double hydroxide, Bi₂MoO₆, Nanocomposite, Active site, Visible-light photodegradation, Heterojunction

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郁桂云,胡丰献,程伟伟,韩字童,刘超,戴勇. ZnCuAl-LDH/Bi₂MoO₆纳米复合材料的构建及其可见光催化降解性能[J]. 物理化学学报, 2020, 36(7), 1911016. doi: 10.3866/PKU.WHXB201911016

Yu Guiyun,Hu Fengxian,Cheng Weiwei,Han Zitong,Liu Chao,Dai Yong. ZnCuAl-LDH/Bi₂MoO₆ Nanocomposites with Improved Visible Light-Driven Photocatalytic Degradation[J]. Acta Physico-Chimica Sinica 2020, 36(7), 1911016. doi: 10.3866/PKU.WHXB201911016

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201911016

https://www.whxb.pku.edu.cn/CN/Y2020/V36/I7/1911016

图/表 9

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ZnCuAl-LDH/Bi₂MoO₆纳米复合材料的构建及其可见光催化降解性能

ZnCuAl-LDH/Bi₂MoO₆ Nanocomposites with Improved Visible Light-Driven Photocatalytic Degradation

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