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Improved photocatalytic performance of acetaldehyde degradation via crystal plane regulation on truncated octahedral CeO2

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Abstract

In this study, the truncated octahedral CeO2 (CeO2-to) with special morphology was prepared by the solvothermal method with oleic acid (OA) and oleamine (OM) as the morphology-directing agents. High-resolution transmission electron microscopy (HRTEM) results show that CeO2-to exposes composite {100} and {111} facets, while CeO2 cubic (CeO2-c) and CeO2 octahedral (CeO2-o) only expose single crystal facets of {100} plane and {111} plane, respectively. Interestingly, this CeO2-to photocatalyst exhibits remarkable photooxidation performance of gaseous acetaldehyde (CH3CHO) degradation, in which CO2 generation value reaches 1.78 and 7.97-times greater than that of CeO2-c and CeO2-o, respectively. In addition, the active species trapping experiment signifies that superoxide (·O2−) and holes (h+) are the main reactive substances during the CH3CHO degradation process, and the electron paramagnetic resonance (EPR) spectra indicates that the former is the major contributor. Notably, the electron transfer mechanism between CeO2-to {100} and {111} facets and the surface oxygen adsorption ability are revealed via density functional theory (DFT) calculations. It is also confirmed that {100} facets are more conducive to the absorption of acetaldehyde than {111} facets. Finally, a reasonable mechanism for improved photocatalytic CH3CHO degradation on CeO2-to is proposed based on relevant experiments and DFT calculations. This study demonstrates that the systematic development of surface homojunction structured photocatalysts can efficiently increase the degradation activity for volatile organic compounds (VOCs). It also offers additional direction for optimizing the photocatalytic activity of other cerium-based photocatalysts.

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摘要

本研究以油酸和油胺为形貌修饰剂，采用溶剂热法制备了具有特殊形态的截断八面体CeO2 (CeO2-to) 。高分辨率透射电镜(HRTEM)显示，CeO2-to 暴露出{100}和{111}复合晶面，而CeO2立方体(CeO2-c) 和CeO2 八面体(CeO2-o) 分别只暴露出{100} 面和{111} 面的单晶面。值得注意的是， CeO2-to 光催化剂对气态乙醛(CH3CHO) 的降解表现出显著的光氧化性能，其CO2 生成值分别是CeO2-c 和CeO2-o 的1.78 倍和7.97 倍。此外，活性物质捕获实验表明，•O2−和h+是CH3CHO 降解过程中的主要活性物质，并且通过电子顺磁共振(EPR)谱显示前者是主要贡献者。同时还通过密度泛函理论(DFT)计算揭示了CeO2-to {100}和{111}表面的电子转移机理和表面氧吸附能力，证实了{100}面比{111}面更有利于乙醛的吸收。最后，通过相关实验和DFT 计算结果的分析，提出了CeO2-to 光催化降解乙醛的合理机理。研究表明，通过系统地开发表面同质结结构的光催化剂，可以有效地提高其对挥发性有机化合物(VOCs) 的降解活性。这也为优化其他铈基光催化剂的光催化活性提供了新的方向。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 21805191 and 22205084), Project funded by China Postdoctoral Science Foundation (No. 2023M741039), Project funded by National & Local Joint Engineering Research Center for Mineral Salt Deep Utilization (SF202303), Project Funded by Yangzhou University (137013308), Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515010982), Shenzhen Stable Support Project (No. 20200812122947002), the Innovative Science and Technology Platform Project of Cooperation between Yangzhou City and Yangzhou University, and Postgraduate Research & Practice Innovation Program of Jiangsu Province (Yangzhou University, No. XKYCX20_014).

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Authors and Affiliations

  1. School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, China

    Bin Xu, Lu Jia, Hui Yang, Yue Wang, Si-Yu Fan & Ming Zhang

  2. College of Environmental Science and Engineering, Yangzhou University, Yangzhou, 225127, China

    Hui Yang

  3. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang , 212000, China

    Sai-Sai Yuan

  4. International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, China

    Qi-Tao Zhang

  5. Department of Applied Chemistry, Faculty of Engineering, Kyushu Institute of Technology, Kitakyushu, 804-8550, Japan

    Hui Yang, Yue Wang & Teruhisa Ohno

  6. National & Local Joint Engineering Research Center for Mineral Salt Deep Utilization, Huaiyin Institute of Technology, Huaian, 223003, China

    Sai-Sai Yuan

  7. School of Materials Science and Engineering, Henan University of Science and Technology, Luoyang, 471000, China

    Sai-Sai Yuan

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Xu, B., Jia, L., Yang, H. et al. Improved photocatalytic performance of acetaldehyde degradation via crystal plane regulation on truncated octahedral CeO2. Rare Met. 43, 2026–2038 (2024). https://doi.org/10.1007/s12598-023-02566-9

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