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Enhanced photocatalytic activity and mechanism of CeO2 hollow spheres for tetracycline degradation

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Abstract

Recently, researchers have focused on designing and fabricating highly efficient catalysts for photocatalytic organic pollutant removal. Herein, CeO2 hollow spheres were prepared through a simple template method followed by calcination at different temperatures for the tetracycline (TC) degradation under simulated solar light illumination. With a calcination temperature ranging from 400 to 800 °C, the as-prepared CeO2 hollow structure annealed at 600 °C (C600) exhibited the best degradation performance with a degradation rate constant of 0.066 min−1, which was about six and five times higher than those of the uncalcined sample (C0) and the sample calcined at 800 °C (C800), respectively. Moreover, sample C600 was also superior to the CeO2 solid particle photocatalyst. The characterisation results showed that the improved photocatalytic performance was mainly ascribed to the synergistic effect of large specific surface areas, high crystallisation and excellent light scattering ability. Furthermore, the results of active species trap** experiments demonstrated that the superoxide anion (•O2−) radical and hole (h+) played dominant roles in TC degradation. Subsequently, the possible TC degradation pathways and photocatalytic mechanism of CeO2 hollow spheres were proposed on the basis of high-performance liquid chromatography–mass spectrometry analysis, main active species and band edge positions of CeO2. The results of this study provide a basis for designing and exploring hollow structure catalysts for energy conversion and environmental remediation.

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摘要

**年来, 设计和制备高活性光催化剂应用于降解有机污染物领域受到了研究者们的广泛关注。在此, 本工作利用模板法和高温煅烧法制备了二氧化铈空心球, 并在模拟太阳光照射下将其应用于降解四环素。实验结果表明:在400-800 °C 煅烧温度范围内, 600 °C煅烧条件下所得的样品 (C600) 表现出最佳光催化性能, 其降解速率常数为0.066 min-1, 这一降解速率常数值分别为未煅烧二氧化铈空心球 (C0) 的6倍和800 °C煅烧条件下制得二氧化铈空心球(C800)的5倍。同时, 该催化剂的光催化性能远优于二氧化铈纳米颗粒。该增**效应得益于C600较大的比表面积、高的结晶性、良好的光子捕获能力。活性物种捕获实验揭示了二氧化铈空心球光催化降解四环素过程中主要活性物种为•O2−和 h+。此外, 通过对反应过程中间体的测试和二氧化铈带隙的表征, 提出了四环素在光催化降解过程中的反应路径。本工作为设计和探索空心结构催化剂应用于环境修复方面奠定了基础。

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Acknowledgments

This work was financially supported by the National Natural Science Foundation of China (Nos. 51961135303, 51932007, 21871217, U1905215 and U1705251), the Innovative Research Funds of Foshan **anhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory (No. XHD2020-001), the National Postdoctoral Program for Innovative Talents (No. BX20200261), China Postdoctoral Science Foundation (No. 2020M682501) and Dean Research Fund (Nos. 04530 and 04554), EdUHK.

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  1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, China

    Dan Wang, Fang-**n Yin, Bei Cheng, Yang **a & Jia-Guo Yu

  2. School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Jia-Guo Yu

  3. Department of Science and Environmental Studies, The Education University of Hong Kong, Tai Po, 999077, Hong Kong, China

    Wing-Kei Ho

  4. State Key Laboratory of Marine Pollution, City University of Hong Kong, Kowloon, 999077, Hong Kong, China

    Wing-Kei Ho

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  1. Dan Wang
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Wang, D., Yin, FX., Cheng, B. et al. Enhanced photocatalytic activity and mechanism of CeO2 hollow spheres for tetracycline degradation. Rare Met. 40, 2369–2380 (2021). https://doi.org/10.1007/s12598-021-01731-2

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