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Mechanistic insight into the framework methylation of H-ZSM-5 for varying methanol loading and Si/Al ratio using first principles molecular dynamics simulations

Nastase, Stefan A. F., Cnudde, Pieter, Vanduyfhuys, Louis, De Wispelaere, Kristof, Van Speybroeck, Veronique, Catlow, C. Richard A. and Logsdail, Andrew J. 2020. Mechanistic insight into the framework methylation of H-ZSM-5 for varying methanol loading and Si/Al ratio using first principles molecular dynamics simulations. ACS Catalysis 10 , pp. 8904-8915. 10.1021/acscatal.0c01454
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Abstract

The methanol-to-hydrocarbons process is known to proceed autocatalytically in H-ZSM-5 after an induction period where framework methoxy species are formed. In this work, we provide mechanistic insight into the framework methylation within H-ZSM-5, at high methanol loadings and varying acid site density, by means of first principles molecular dynamics simulations. The molecular dynamics simulations show that stable methanol clusters form in the zeolite pores, and these clusters commonly deprotonate the active site, however the cluster size is dependent on temperature and acid site density. Enhanced sampling molecular dynamics simulations give evidence that the barrier for methanol conversion is significantly affected by the neighbourhood of an additional acid site, suggesting that cooperative effects influence methanol clustering and reactivity. The insights obtained are important steps in optimising the catalyst and engineering the induction period of the methanol-to-hydrocarbons process.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: American Chemical Society
ISSN: 2155-5435
Date of First Compliant Deposit: 13 July 2020
Date of Acceptance: 12 July 2020
Last Modified: 31 Aug 2020 16:46
URI: http://orca.cf.ac.uk/id/eprint/133391

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