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Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol.

Authors
  • Meng, Lingqian1
  • Zhu, Xiaochun1
  • Hensen, Emiel J M1
  • 1 Inorganic Materials Chemistry, Schuit Institute of Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands. , (Netherlands)
Type
Published Article
Journal
ACS Catalysis
Publisher
American Chemical Society
Publication Date
Apr 07, 2017
Volume
7
Issue
4
Pages
2709–2719
Identifiers
DOI: 10.1021/acscatal.6b03512
PMID: 28413693
Source
Medline
Keywords
License
Unknown

Abstract

Fe/ZSM-5 nanosheet zeolites of varying thickness were synthesized with di- and tetraquaternary ammonium structure directing agents and extensively characterized for their textural, structural, and catalytic properties. Introduction of Fe3+ ions in the framework of nanosheet zeolites was slightly less effective than in bulk ZSM-5 zeolite. Steaming was necessary to activate all catalysts for N2O decomposition and benzene oxidation. The higher the Fe content, the higher the degree of Fe aggregation was after catalyst activation. The degree of Fe aggregation was lower when the crystal domain size of the zeolite or the Fe content was decreased. These two parameters had a substantial influence on the catalytic performance. Decreasing the number of Fe sites along the b-direction strongly suppressed secondary reactions of phenol and, accordingly, catalyst deactivation. This together with the absence of diffusional limitations in nanosheet zeolites explains the much higher phenol productivity obtainable with nanostructured Fe/ZSM-5. Steamed Fe/ZSM-5 zeolite nanosheet synthesized using C22-6-3·Br2 (domain size in b-direction ∼3 nm) and containing 0.24 wt % Fe exhibited the highest catalytic performance. During the first 24 h on stream, this catalyst produced 185 mmolphenol g-1. Calcination to remove the coke deposits completely restored the initial activity.

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