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

[Image: see text] 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 Fe(3+) ions in the framework of nanosheet zeoli...

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Autores principales: Meng, Lingqian, Zhu, Xiaochun, Hensen, Emiel J. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2017
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5389689/
https://www.ncbi.nlm.nih.gov/pubmed/28413693
http://dx.doi.org/10.1021/acscatal.6b03512
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author Meng, Lingqian
Zhu, Xiaochun
Hensen, Emiel J. M.
author_facet Meng, Lingqian
Zhu, Xiaochun
Hensen, Emiel J. M.
author_sort Meng, Lingqian
collection PubMed
description [Image: see text] 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 Fe(3+) 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 N(2)O 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 C(22-6-3)·Br(2) (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 mmol(phenol) g(–1). Calcination to remove the coke deposits completely restored the initial activity.
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spelling pubmed-53896892017-04-13 Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol Meng, Lingqian Zhu, Xiaochun Hensen, Emiel J. M. ACS Catal [Image: see text] 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 Fe(3+) 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 N(2)O 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 C(22-6-3)·Br(2) (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 mmol(phenol) g(–1). Calcination to remove the coke deposits completely restored the initial activity. American Chemical Society 2017-03-10 2017-04-07 /pmc/articles/PMC5389689/ /pubmed/28413693 http://dx.doi.org/10.1021/acscatal.6b03512 Text en Copyright © 2017 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Meng, Lingqian
Zhu, Xiaochun
Hensen, Emiel J. M.
Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol
title Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol
title_full Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol
title_fullStr Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol
title_full_unstemmed Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol
title_short Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol
title_sort stable fe/zsm-5 nanosheet zeolite catalysts for the oxidation of benzene to phenol
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5389689/
https://www.ncbi.nlm.nih.gov/pubmed/28413693
http://dx.doi.org/10.1021/acscatal.6b03512
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