Activation of n-pentane while prolonging HZSM-5 catalyst lifetime during its combined reaction with methanol or dimethyl ether

Tomás Cordero-Lanzac, Cristina Martínez, Andrés T. Aguayo, Pedro Castaño, Javier Bilbao, Avelino Corma

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21 Scopus citations

Abstract

This work explores the synergies during combined reactions of n-pentane (nC5) with oxygenates (methanol or dimethyl ether, OX). The experimental runs have been carried out in a packed bed reactor at 500 °C, using a high silica HZSM-5 zeolite-based catalyst with different oxygenate-to-n-pentane (OX/nC5) ratios in the feed. A significant enhancement of the n-pentane conversion occurs for low OX/nC5 ratios in the feed (0.1−0.25), especially when using dimethyl ether (DME). In addition, the presence of n-pentane reduces the rate of catalyst deactivation by coking during the conversion of oxygenates. These results have been explained on the grounds of a mechanistic interaction between the reactants: (1) the fast formation of methoxy and olefin intermediates from oxygenates, particularly from DME, could explain the promotion of n-pentane cracking, by facilitating the activation of the alkane by hydrogen transfer reactions; (2) the attenuation of deactivation during the conversion of oxygenates could be related to a lower extent of the arene cycle in the dual-cycle mechanism (limiting the polymethylbenzene formation). The analyses of used catalysts by means of temperature-programmed oxidation and confocal fluorescence microscopy have pointed out the higher reactivity of DME than that of methanol also for yielding coke structures.
Original languageEnglish (US)
JournalCatalysis Today
DOIs
StatePublished - Sep 18 2020

Bibliographical note

KAUST Repository Item: Exported on 2020-10-16
Acknowledgements: TC-L, ATA, PC and JB acknowledge the financial support received by the Spanish Ministry of Economy and Competitiveness with some ERDF funds (CTQ2016-77812-R,CTQ2016-79646-P), theBasque Government (IT1218-19) and theEuropean Commission(HORIZON H2020-MSCA RISE-2018. Contract No. 823745). TC-L also acknowledges the Spanish Ministry of Education, Culture and Sport for the award of the FPU grant (FPU15-01666) and the additional mobility grant (EST17-00094). CM and AC acknowledge national and regional funding (MICINN/GVA) through ‘Severo Ochoa” (SEV-2016-0683), RTI2018-101033-B-I00 and AICO/2019/060 and financial support from EU byERC-AdG-2014-671093(SynCatMatch) and from the Fundación Ramón Arecesthrough a research contract of the “Life and Materials Science” program. The authors also thank Dr. Ricardo Andrade of the SGIker of UPV/EHU for the support provided with the CFM technique.

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