Nastase, Stefan A. F., Cnudde, Pieter, Vanduyfhuys, Louis, De Wispelaere, Kristof, Van Speybroeck, Veronique, Catlow, C. Richard A. ORCID: https://orcid.org/0000-0002-1341-1541 and Logsdail, Andrew J. ORCID: https://orcid.org/0000-0002-2277-415X 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 |
Preview |
PDF
- Accepted Post-Print Version
Download (871kB) | Preview |
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) Advanced Research Computing @ Cardiff (ARCCA) |
Publisher: | American Chemical Society |
ISSN: | 2155-5435 |
Date of First Compliant Deposit: | 13 July 2020 |
Date of Acceptance: | 12 July 2020 |
Last Modified: | 14 Nov 2023 16:41 |
URI: | https://orca.cardiff.ac.uk/id/eprint/133391 |
Citation Data
Cited 21 times in Scopus. View in Scopus. Powered By Scopus® Data
Actions (repository staff only)
Edit Item |