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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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