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Highly active CeO2 hollow-shell spheres with Al doping

铝掺杂氧化铈多壳层空心球的可控合成及其催化应用

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Abstract

Metal oxide hollow structures are of great interest in many current and emerging areas of technology. This paper presents a facile and controlled protocol for the synthesis of Al-doped CeO2 hollow-shell spheres (CHS), where the dopant confers enhanced stability and activity to the material. These Al-doped CeO2 hollow-shell spheres (ACHS) possess a controllable shell number of up to three, where the sizes of the exterior, middle, and interior spheres were about 250‒100 nm,150‒50 nm, and 40‒10 nm, respectively, and the average shell thickness was ~15 nm. The thermal stability of the ACHS structure was enhanced by the homogeneous incorporation of Al atoms, andmore active oxygen species were present compared with those in the non-doped congener. Au NPs supported on ACHS (Au/ACHS) showed superior catalytic performance for the reduction of p-nitrophenol. For the same Au NP content, the reaction rate constant (k) of the Au/ACHS was nearly twice that of the non-doped Au/CHS, indicating that Al doping is promising for improving the performance of inert or unstable oxides as catalyst supports.

摘要

本文利用多孔碳球为模板, 通过竞争吸附控制煅烧法制备了铝掺杂的氧化铈多壳层空心球材料. 通过XRD、SEM、TEM对所得材料的结构、表面形貌以及热稳定性能进行了表征, 结果表明该方法制备的不同掺杂比例的多壳层空心球均一分散, 铝原子被均匀地分布到氧化铈的晶格中, 使其热稳定性得到提高. XPS结果表明铝的掺杂大大提高了材料中三价铈和表面氧空位的比例, 所以当其被作为催化剂载体时, 负载的金纳米粒子更加分散且与载体结合作用更强. 将该催化剂应用于硝基苯酚加氢反应, 其催化活性比未掺杂铝的样品提高了一倍.本文研究结果表明铝掺杂可以有效提高氧化铈催化剂的稳定性和活性; 竞争吸附控制煅烧法是制备空心掺杂材料的一种简单实用的方法.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51472025 and 21671016) and Beijing Nova Programme Interdisciplinary Cooperation Project.

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Physical Chemistry, University of Science and Technology Beijing, Beijing, 100083, China

    Zumin Wang  (王祖民), Shuaiyu Jiang  (姜帅宇), Yanhui Li  (李彦辉), Pengfei Xu  (徐鹏飞), Kun Zhao  (赵昆), Lingbo Zong  (宗玲博) & Ranbo Yu  (于然波)

  2. Centre for Future Materials, University of Southern Queensland, Queensland, 4350, Australia

    Hao Wang  (王浩) & Ranbo Yu  (于然波)

Authors
  1. Zumin Wang  (王祖民)
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  7. Hao Wang  (王浩)
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  8. Ranbo Yu  (于然波)
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Corresponding author

Correspondence to Ranbo Yu  (于然波).

Additional information

Author contributions Wang Z designed and engineered the samples; Jiang S and Li Y performed the experiments;Wang Z wrote the paper with support from Jiang S. All authors contributed to the general discussion.

Conflict of interest The authors declare that they have no conflict of interest.

Supplementary information Supporting data are available in the online version of the paper.

Zumin Wang received his BE degree from the School of Metallurgical and Ecological Engineering, the University of Science and Technology, Beijing (USTB) in 2012. He is currently studying for his PhD degree under the supervision of Prof. Ranbo Yu from the Laboratory of Physical Chemistry of Materials Preparation at the Department of Physical Chemistry, USTB.His current research interests are focused on the design and synthesis ofmicro-/nanostructured functional inorganic nanomaterials for catalysis.

Shuaiyu Jiang received his BE degree from the University of Science and Technology Liaoning (2013) and MSc from the USTB (2016). He is currently a PhD candidate at the Griffith University. His current research interest is focused on the synthesis of micro-/nanostructured photocatalyst.

Ranbo Yu received her BSc and MSc degrees at Jilin University (1994 and 1997) and PhD at Yamanashi University (2002). As a postdoctoral researcher she worked in Kyoto University (JSPS fellow) and the University of Houston in 2002 and 2003. She currently holds a professor position at the Department of Physical Chemistry, USTB. Her research interests focus on the development of micro-/nanostructured functional inorganic materials and their applications in catalysis.

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Wang, Z., Jiang, S., Li, Y. et al. Highly active CeO2 hollow-shell spheres with Al doping. Sci. China Mater. 60, 646–653 (2017). https://doi.org/10.1007/s40843-017-9042-0

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