Advanced oxidation process for coke removal: A systematic study of hydrogen peroxide and OH-derived-Fenton radicals of a fouled zeolite

[Display omitted] •Advanced oxidation processes have been applied on a coked zeolite.•Structure and texture were preserved, while acidity was improved.•Complete catalyst activity recovery was achieved.•Water treatment, followed by H2O2 and finally Fenton process are recommended as methodology guidel...

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Veröffentlicht in:Applied catalysis. A, General General, 2018-07, Vol.562, p.215-222
Hauptverfasser: Morales, María V., Góra-Marek, Kinga, Musch, Hermen, Pineda, Antonio, Murray, Blaine, Stefanidis, Stelios, Falco, Lorena, Tarach, Karolina, Ponomareva, Ekaterina, Marsman, Jan Henk, Melián-Cabrera, Ignacio
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container_title Applied catalysis. A, General
container_volume 562
creator Morales, María V.
Góra-Marek, Kinga
Musch, Hermen
Pineda, Antonio
Murray, Blaine
Stefanidis, Stelios
Falco, Lorena
Tarach, Karolina
Ponomareva, Ekaterina
Marsman, Jan Henk
Melián-Cabrera, Ignacio
description [Display omitted] •Advanced oxidation processes have been applied on a coked zeolite.•Structure and texture were preserved, while acidity was improved.•Complete catalyst activity recovery was achieved.•Water treatment, followed by H2O2 and finally Fenton process are recommended as methodology guidelines. The regeneration process of a fouled catalyst typically involves treatments at high temperature which often cause irreversible damages on the catalyst’s properties. In this work, Fenton chemistry-derived OH• species, and H2O2, are proposed as oxidizing agents to reactivate a porous catalyst at mild conditions, below 100 °C. The chosen catalyst is a microporous ZSM-5 zeolite, which is a challenging candidate due to the mass transfer limitations with possible recombination of the hydroxyl radicals; thereby being an obstacle to oxidize organics occluded in the micropores. The organics deposition over a ZSM-5 zeolite during the D-glucose dehydration reaction was confirmed by a number of characterization techniques, which revealed a considerable decrease in the surface area, pore volume and acid site density in the fouled catalyst. By properly selecting the regeneration conditions, reactivation via Fenton or H2O2 was highly effective in terms of removal of the organics as well as recovery of the initial catalytic activity. The properties of the H2O2 treated-zeolite, the optimal treatment in this case study, were preserved with similar structural and textural features and improved acidity. Hot water extraction was ineffective to remove the humins from ZSM-5. Mechanistically, the presence of Fe impurities in the zeolite structure did not allow to discriminate between a homo, heterogeneous, or a direct H2O2 pathway, or a combination of them. The exhibited conversion by the regenerated zeolite was comparable to that of the fresh one.
doi_str_mv 10.1016/j.apcata.2018.06.008
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By properly selecting the regeneration conditions, reactivation via Fenton or H2O2 was highly effective in terms of removal of the organics as well as recovery of the initial catalytic activity. The properties of the H2O2 treated-zeolite, the optimal treatment in this case study, were preserved with similar structural and textural features and improved acidity. Hot water extraction was ineffective to remove the humins from ZSM-5. Mechanistically, the presence of Fe impurities in the zeolite structure did not allow to discriminate between a homo, heterogeneous, or a direct H2O2 pathway, or a combination of them. 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ispartof Applied catalysis. A, General, 2018-07, Vol.562, p.215-222
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source Elsevier ScienceDirect Journals
subjects Activation
Catalysis
Catalysts
Catalytic activity
Coke
Dehydration
Feature extraction
Fenton chemistry
Fouling
Hydrogen peroxide
Hydroxyl radicals
Mass transfer
Organic chemistry
Oxidation
Oxidizing agents
Reactivation
Regeneration
Zeolites
title Advanced oxidation process for coke removal: A systematic study of hydrogen peroxide and OH-derived-Fenton radicals of a fouled zeolite
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