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The selective deposition of Fe species inside ZSM-5 for the oxidation of cyclohexane to cyclohexanone

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Abstract

The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions. Because of the complex distribution of iron location on the support, the selectivity is always low. Here, we report a general strategy to selectively deposit highly-dispersed FeOx into the micropore of ZSM-5 by atomic layer deposition (ALD). The framework of ZSM-5 and the Brønsted acid sites are intact during ALD, and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5. Besides, more Fe-O-Si bonds are formed over FeOx/ZSM-5 with a low loading of Fe, while FeOx nanoparticles are generated at high Fe loading. They cannot be realized by the traditional solution method. The obtained FeOx/ZSM-5 catalysts perform high selectivity of cyclohexanone (92%–97%), and ALD cycle numbers of FeOx control the activity. Compared with the Fe nanoparticles, the Fe-O-Si species performs higher turnover frequency and stability in the oxidation reaction.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21872160, U1832208), the National Science Fund for Distinguished Young Scholars (21825204), the National Key R&D Program of China (2017YFA0700101 and 2018YFB1501602), the Youth Innovation Promotion Association CAS (2017204), and Natural Science Foundation of Shanxi Province (201901D211591).

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Authors and Affiliations

  1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China

    Liming Zhai, Bin Zhang, Haojie Liang, Huibin Wu, Xinchun Yang, Gen Luo, Shichao Zhao & Yong Qin

  2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China

    Liming Zhai, Bin Zhang, Haojie Liang, Huibin Wu, Xinchun Yang, Gen Luo & Yong Qin

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  1. Liming Zhai
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  2. Bin Zhang
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  3. Haojie Liang
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  6. Gen Luo
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  7. Shichao Zhao
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  8. Yong Qin
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Correspondence to Bin Zhang.

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The authors declare no conflict of interest.

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The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Zhai, L., Zhang, B., Liang, H. et al. The selective deposition of Fe species inside ZSM-5 for the oxidation of cyclohexane to cyclohexanone. Sci. China Chem. 64, 1088–1095 (2021). https://doi.org/10.1007/s11426-020-9968-x

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  • DOI: https://doi.org/10.1007/s11426-020-9968-x

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