The Influence of Mesopore Architecture in Hierarchical H-ZSM-5 on n-Butanol Dehydration

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Titel: The Influence of Mesopore Architecture in Hierarchical H-ZSM-5 on n-Butanol Dehydration
Autoren: Phebe Lemaire, Arno de Reviere, Dhanjay Sharma, Valérie Ruaux, Jaouad Al Atrach, Valentin Valtchev, Joris Thybaut, Maarten Sabbe, An Verberckmoes
Quelle: ACS ENGINEERING AU
Verlagsinformationen: American Chemical Society (ACS), 2025.
Publikationsjahr: 2025
Schlagwörter: platelike H-ZSM-5, Technology and Engineering, desilication, ACID SITES, B-AXIS, DESILICATION, hierarchization, ZSM-5 ZEOLITES, BUTENE ISOMERS, CATALYTIC CRACKING, Chemistry, AL DISTRIBUTION, butanol dehydration, MECHANISTIC INSIGHTS, zeolite, MFI ZEOLITES, COKE FORMATION
Beschreibung: Zeolites are among the most widely employed catalysts in the (petro-)chemical industry. However, due to their elaborate microporous network, they are prone to diffusion limitations and deactivation. Several modification methods have been proposed to overcome these limitations, each exhibiting their benefits. In this work, two of the most promising strategies were combined, i.e., limiting the length of one of the crystal axes during synthesis to achieve a platelike morphology and introducing mesoporosity, creating a hierarchical platelike H-ZSM-5. The platelike morphology was obtained by adding urea as a growth modifier to the synthesis mixture, and mesopores were introduced in the platelike H-ZSM-5 through etching with a NaOH/TPAOH mixture. As a benchmark, the same etching procedure was applied to a commercial ZSM-5 counterpart. These materials were tested in the n-butanol dehydration, where the platelike morphology exhibited an improved catalytic performance, significantly increasing the activity per acid site and stability, and slightly increasing the selectivity toward the butenes. The generation of mesopores in commercial ZSM-5 also increased the activity per acid site but reduced the catalyst's stability, likely due to an increased amount of Lewis acid sites upon etching. When applying the same modification method to the platelike H-ZSM-5, much larger mesopores and some macropores were observed. These further increased the stability of the catalyst but barely affected the activity per acid site, presumably due to the already optimized catalytic performance of the platelike H-ZSM-5.
Publikationsart: Article
Dateibeschreibung: application/pdf
Sprache: English
ISSN: 2694-2488
DOI: 10.1021/acsengineeringau.5c00033
Zugangs-URL: http://hdl.handle.net/1854/LU-01K3RA65J9MCNVQ3QSRTDDRVMC
https://biblio.ugent.be/publication/01K3RA65J9MCNVQ3QSRTDDRVMC
http://doi.org/10.1021/acsengineeringau.5c00033
https://biblio.ugent.be/publication/01K3RA65J9MCNVQ3QSRTDDRVMC/file/01K3RA8Y0N1VVP2GVYC0MTF1TX
Rights: CC BY NC ND
Dokumentencode: edsair.doi.dedup.....b10118d33a9fb90493c20cf4c72acbd2
Datenbank: OpenAIRE
Beschreibung
Abstract:Zeolites are among the most widely employed catalysts in the (petro-)chemical industry. However, due to their elaborate microporous network, they are prone to diffusion limitations and deactivation. Several modification methods have been proposed to overcome these limitations, each exhibiting their benefits. In this work, two of the most promising strategies were combined, i.e., limiting the length of one of the crystal axes during synthesis to achieve a platelike morphology and introducing mesoporosity, creating a hierarchical platelike H-ZSM-5. The platelike morphology was obtained by adding urea as a growth modifier to the synthesis mixture, and mesopores were introduced in the platelike H-ZSM-5 through etching with a NaOH/TPAOH mixture. As a benchmark, the same etching procedure was applied to a commercial ZSM-5 counterpart. These materials were tested in the n-butanol dehydration, where the platelike morphology exhibited an improved catalytic performance, significantly increasing the activity per acid site and stability, and slightly increasing the selectivity toward the butenes. The generation of mesopores in commercial ZSM-5 also increased the activity per acid site but reduced the catalyst's stability, likely due to an increased amount of Lewis acid sites upon etching. When applying the same modification method to the platelike H-ZSM-5, much larger mesopores and some macropores were observed. These further increased the stability of the catalyst but barely affected the activity per acid site, presumably due to the already optimized catalytic performance of the platelike H-ZSM-5.
ISSN:26942488
DOI:10.1021/acsengineeringau.5c00033