利用Ag/CeO2的缺陷增强水中抗生素的光催化降解：结构特征、机理和降解途径的深入研究

IF 5.5 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Advances Pub Date : 2025-01-12 DOI:10.1016/j.ceja.2025.100706

Ajit Kumar Dhanka , Emerson C. Kohlrausch , Raghabendra Samantray , Vinod Kumar , Balaram Pani , Nityananda Agasti

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引用次数: 0

摘要

制备了一种高效稳定的光催化降解水中抗生素的ceo2基材料。在这项研究中，我们研究了Ag/CeO2纳米复合材料中由于Ag和CeO2之间的金属负载相互作用而导致的缺陷。本文通过在CeO2表面掺入Ag来引入氧空位。值得注意的是，在CeO2中加入Ag使带隙能降低到2.90 eV，同时Ce3+含量增加，这与氧空位的增加有关。x射线光电子能谱（XPS）、拉曼和EPR研究证实了Ag与CeO2相互作用导致CeO2表面氧空位的增加。Ag/CeO2中的氧空位作为光生电子的捕获位点，成功地抑制了光生电子和空穴对的重组，从而提高了Ag/CeO2纳米复合材料的催化活性。Ag/CeO2纳米复合材料表现出比原始CeO2更好的催化性能，这是由于纳米复合材料中氧空位的增强。我们研究了银（Ag）对Ag/CeO2中氧空位增加的影响。通过捕集实验确定参与光催化降解过程的活性物质。基于对纳米复合材料表征技术和光催化实验结果的批判性分析，提出了一种合理的机理。基于高分辨率质谱分析，提出了环丙沙星及其降解中间体的可能降解途径。本研究揭示了缺陷CeO2的结构特征，深入了解了环丙沙星的光催化机理和降解途径，为探索其他用于催化应用的铈基纳米复合材料提供了基础。

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Harnessing defects in Ag/CeO2 for enhanced photocatalytic degradation of antibiotic in water: Structural characteristics, in-depth insights on mechanism, degradation pathway

A highly efficient and stable CeO₂-based material has been developed for photocatalytic degradation of antibiotics in water. In this study, we investigated the defects due to metal-support interaction between Ag and CeO₂ in the Ag/CeO₂ nanocomposites. Here we introduced oxygen vacancies in CeO₂ by incorporating Ag on the surface of CeO_2. Notably, the addition of Ag to CeO₂ reduces the band gap energy to 2.90 eV, accompanied by an increase in Ce³⁺ content which is correlated with an increase in oxygen vacancies. X-ray photoelectron spectroscopy (XPS), Raman and EPR studies substantiated the increase in surface oxygen vacancies in CeO₂ induced by the interaction between Ag and CeO₂. Oxygen vacancies in Ag/CeO₂ act as trapping sites for photogenerated electrons and successfully restrain the recombination of photogenerated electron and hole pairs, thereby exhibiting improved catalytic activity of Ag/CeO₂ nanocomposites. Ag/CeO₂ nanocomposites exhibited better catalytic performance than pristine CeO₂, which is attributed to the enhanced oxygen vacancies in the nanocomposites. We investigated the effect of silver (Ag) on increasing oxygen vacancies in Ag/CeO₂.Trapping experiments were conducted to identify the reactive species participating in the photocatalytic degradation process. A plausible mechanism is proposed based on critical analysis of the results from the characterization techniques of the nanocomposites and photocatalytic experiments. The possible degradation pathways for Ciprofloxacin along with the degradation intermediates have been proposed based on High resolution mass spectroscopy (HRMS) analysis. This study provides insights on structural characteristics of defective CeO₂, in-depth photocatalytic mechanism and degradation pathway of ciprofloxacin, that could facilitate the exploration of other ceria-based nanocomposites for catalytic applications.

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