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Photocatalytic in situ H2O2 production and activation for enhanced ciprofloxacin degradation over CeO2-Co3O4/g-C3N4: key role of CeO2

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Abstract

The abused ciprofloxacin antibiotics have caused significant environmental damage. Although oxidative degradation of ciprofloxacin exhibits promising efficacy, it often entails excessive energy consumption. Hence, it is necessary to explore an effective and ecologically sustainable degradation strategy. Herein, we demonstrated that g-C3N4 decorated with the coordinated CeO2 and Co3O4 (CeO2-Co3O4/CN) exhibited effective ciprofloxacin photodegradation via in situ H2O2 production and activation mechanism. Results indicate that the introduced CeO2 enhances the transference of photogenerated electrons to O2 by adjusting the oxygen vacancy of photocatalyst, thereby increasing the generation of superoxide radicals, which in turn generate H2O2, resulting in a 22.4-fold increase in H2O2 generation over g-C3N4. Moreover, the in situ H2O2 generation facilitated by CeO2 is confirmed to be essential for ciprofloxacin degradation via CeO2-Co3O4/CN, as it provides enough oxidant for Co3O4 to activate into hydroxyl radicals for the pollutants degradation. Ultimately, CeO2-Co3O4/CN achieves a ciprofloxacin degradation ratio of 97.7% within 80 min. This study introduces a novel approach that combines H2O2 generation and activation, offering an innovative perspective for achieving clean and efficient purification of antibiotic-contaminated water.

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摘要

环丙沙星(CIP)一类抗生素的滥用对环境造成了严重的危害, 而氧化降解CIP虽然效果明显但通常会产生较高能耗, 所以探究一种高效清洁的降解方法迫在眉睫。本研究提出以氮化碳为光敏载体, 通过在其表面负载和协调CeO2和Co3O4两种活性组分, 最终成功合成能够串联H2O2生成和活化反应的光催化剂(CeO2-Co3O4/CN), 并达到高效降解CIP的目的。结果表明, 得益于CeO2能够富集光生电子的性质及其自身对氧气的吸附能力, 催化剂的H2O2生成效果比氮化碳提高了22.41倍, 并证实上述CeO2特性是复合材料能够高效降解污染物的关键因素。此外, 负载Co3O4则有利于高效活化生成的H2O2, 并且证实了CeO2-Co3O4/CN能够协调进行这两步反应, 最终在80 min内达到97.7%的CIP降解率。本研究提出了一种串联H2O2生成反应和活化反应的新方法, 为清洁高效降解水中抗生素提供了一种新的思路。

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Acknowledgements

This study was financially supported by Shandong Provincial Natural Science Foundation (No. ZR2021QB123), Liaocheng University Start-up Fund for Doctoral Scientific Research (No. 318052017) and the Open Fund of State Key Lab of Pollution Control and Resource Reuse Research, China (No. PCRRF20002). We would like to thank Liaocheng YiLu Advanced Materials Co. Ltd for assistance in photocatalyst synthesis and language editing.

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Authors and Affiliations

  1. Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng, 252059, China

    Hong-Jie Zhu, Yi-Kai Yang & Hai-Tao Zhao

  2. College of Ecology and Environment, Anhui Normal University, Wuhu, 241002, China

    Ming-Hui Li

  3. Liaocheng YiLu Advanced Materials Co., Ltd, Liaocheng, 252000, China

    Lu-Ning Zou

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Zhu, HJ., Yang, YK., Li, MH. et al. Photocatalytic in situ H2O2 production and activation for enhanced ciprofloxacin degradation over CeO2-Co3O4/g-C3N4: key role of CeO2. Rare Met. 43, 2695–2707 (2024). https://doi.org/10.1007/s12598-023-02583-8

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