Fabrication and catalytic performance of meso-ZSM-5 zeolite encapsulated ferric oxide nanoparticles for phenol hydroxylation

Abstract

An encapsulation-structured Fe₂O₃@meso-ZSM-5 (Fe@MZ5) was fabricated by confining Fe₂O₃ nanoparticles (ca. 4 nm) within the ordered mesopores of hierarchical ZSM-5 zeolite (meso-ZSM-5), with ferric oleate and amphiphilic organosilane as the iron source and meso-porogen, respectively. For comparison, catalysts with Fe₂O₃ (ca. 12 nm) encapsulated in intra-crystal holes of meso-ZSM-5 and with MCM-41 or ZSM-5 phase as the shell were also prepared via sequential desilication and recrystallization at different pH values and temperatures. Catalytic phenol hydroxylation performance of the as-prepared catalysts using H₂O₂ as oxidant was compared. Among the encapsulation-structured catalysts, Fe@MZ5 showed the highest phenol conversion and hydroquinone selectivity, which were enhanced by two times compared to the Fe-oxide impregnated ZSM-5 (Fe/Z5). Moreover, the Fe-leaching amount of Fe@MZ5 was only 3% of that for Fe/Z5. The influence of reaction parameters, reusability, and ·OH scavenging ability of the catalysts were also investigated. Based on the above results, the structure-performance relationship of these new catalysts was preliminarily described.

Key words： phenol hydroxylation; encapsulation structure; structure-performance relationship; meso-ZSM-5; ferric oxide

Acknowledgements

This work was supported by the National Science Foundation of Jilin Province (No. 20200201208JC).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-020-1972-3 and is accessible for authorized users.

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