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ZnO:Au纳米结构的表面等离子体光催化活性:调控表面等离子体吸收和界面电荷转移机制

Plasmonic photocatalytic activity of ZnO:Au nanostructures: Tailoring the plasmon absorption and interfacial charge transfer mechanism.

作者信息

Raji R, Gopchandran K G

机构信息

Department of Optoelectronics, University of Kerala, Thiruvananthapuram 695581, India.

Department of Optoelectronics, University of Kerala, Thiruvananthapuram 695581, India.

出版信息

J Hazard Mater. 2019 Apr 15;368:345-357. doi: 10.1016/j.jhazmat.2019.01.052. Epub 2019 Jan 18.

Abstract

ZnO:Au nanostructures with tunable surface Plasmon band were synthesizedvia co-precipitation method. X-ray diffraction analysis, high resolution transmission electron microscopy and Raman spectra confirmed the hexagonal wurtzite phase for these ZnO:Au nanostructures with preferential growth along the (101) plane. The selective enhancement in the intensity of Raman band due to the excited free electrons of Au nanoparticles confirmed the incorporation of Au in ZnO matrix. Scanning electron microscopic images showed the transformation of morphology of these nanostructures from rod geometry to rose flower and then to marigold flower-like structures with increase in the Au content. Detailed investigations were carried out to understand the role of plasmons present in the ZnO:Au nanostructures on the photocatalytic degradation of sulforhodamine B under sunlight. It is found that ZnO:Au nanostructures with plasmon band in the close approximation of solar maximum ˜550 nm as catalysts exhibit ultra-fast degradation of the dye. This highly efficient photocatalytic activity of these nanostructures is attributed to the electron scavenging action of Au due to its high electronegativity, enhanced absorption of sunlight due to plasmons, the enhanced surface area of ZnO:Au nanostructures and the formation of Schottky barrier between the Au and ZnO interface. The reusability and photostability of these catalysts were tested through repetitive cycles and demonstrated that these nanostructures can form excellent reusable photocatalysts for the degradation of toxic organic waste in water.

摘要

通过共沉淀法合成了具有可调表面等离子体带的ZnO:Au纳米结构。X射线衍射分析、高分辨率透射电子显微镜和拉曼光谱证实了这些ZnO:Au纳米结构为六方纤锌矿相,且沿(101)面择优生长。由于金纳米颗粒的激发自由电子导致拉曼带强度的选择性增强,证实了金在ZnO基体中的掺入。扫描电子显微镜图像显示,随着金含量的增加,这些纳米结构的形态从棒状转变为玫瑰花状,然后转变为金盏花状结构。进行了详细的研究,以了解ZnO:Au纳米结构中存在的等离子体对阳光下罗丹明B光催化降解的作用。发现等离子体带与太阳最大值~550nm相近的ZnO:Au纳米结构作为催化剂时,染料表现出超快降解。这些纳米结构的这种高效光催化活性归因于金因其高电负性的电子清除作用、等离子体对太阳光的增强吸收、ZnO:Au纳米结构的增大表面积以及Au与ZnO界面处肖特基势垒的形成。通过重复循环测试了这些催化剂的可重复使用性和光稳定性,结果表明这些纳米结构可以形成优异的可重复使用光催化剂,用于降解水中的有毒有机废物。

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