Simultaneous coking and dealumination of zeolite H-ZSM-5 during the transformation of chloromethane into olefins

M. Ibáñez, M. Gamero, J. Ruiz-Martínez, B. M. Weckhuysen, A. T. Aguayo, J. Bilbao, P. Castaño

Research output: Contribution to journalArticlepeer-review

36 Scopus citations

Abstract

The deactivation pathways of a zeolite H-ZSM-5 catalyst containing bentonite and α-Al 2 O 3 as binder material have been studied during the transformation of chloromethane into light olefins, which is considered as a possible step to valorize methane from natural gas. The reactions have been carried out in a fixed bed reactor, feeding pure chloromethane at 400, 425 and 450°C, 1.5 bar and with a space-time of 5.4 (g catalyst ) h (mol CH2 ) -1 for 255 min. The properties of the fresh and spent catalysts have been assessed by several techniques, such as N 2 physisorption, adsorption/desorption of NH 3 , XPS and 29 Si NMR. Additional measurements of the spent catalysts have been performed to study the nature of the deactivating coke species: TG-TPO analysis, SEM, and FT-IR and UV-vis spectroscopy. With the results in hand, two deactivation mechanisms were proposed: irreversible dealumination at temperatures higher than 450°C by HCl and reversible coke fouling, while coke formation results from the condensation of polyalkylbenzenes, which are also intermediates in olefin production. The coke deposits grow in size with the addition of Cl to the carbonaceous structure.

Original languageEnglish (US)
Pages (from-to)296-306
Number of pages11
JournalCatalysis Science and Technology
Volume6
Issue number1
DOIs
StatePublished - Jan 7 2016
Externally publishedYes

ASJC Scopus subject areas

  • Catalysis

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