Jump to main content
Jump to site search
PLANNED MAINTENANCE Close the message box

Scheduled maintenance work on Wednesday 27th March 2019 from 11:00 AM to 1:00 PM (GMT).

During this time our website performance may be temporarily affected. We apologise for any inconvenience this might cause and thank you for your patience.


Issue 5, 2019
Previous Article Next Article

Computational QM/MM investigation of the adsorption of MTH active species in H-Y and H-ZSM-5

Author affiliations

Abstract

The transformation of methanol-to-hydrocarbons (MTH) has significant potential as a route to synthesise low-cost fuels; however, the initial stages of the zeolite catalysed MTH process are not well understood. Here, we use hybrid quantum- and molecular-mechanical (QM/MM) embedded-cluster simulations to develop our understanding of the interaction between methanol and the zeolite catalysts H-ZSM-5, and for comparison, the larger pore H-Y. Energies and structures, calculated using hybrid-level density functional theory (hybrid-DFT) and higher-level correlated methods, are compared with previous experimental and computational results. We show that hydrogen-bonds between methanol adsorbates, formed through polarizable O–H bonds, substantially influence the adsorption energetics, structural parameters and vibrational frequencies. Our observations are extended by considering polar solvent molecules in the environment, with the presence of both water or methanol around the adsorption site leading to barrier-less transfer of the zeolite proton to an adsorbed methanol, which will significantly influence the reactivity of the adsorbed methanol.

Graphical abstract: Computational QM/MM investigation of the adsorption of MTH active species in H-Y and H-ZSM-5

Back to tab navigation

Supplementary files

Publication details

The article was received on 30 Oct 2018, accepted on 20 Dec 2018 and first published on 21 Dec 2018


Article type: Paper
DOI: 10.1039/C8CP06736H
Citation: Phys. Chem. Chem. Phys., 2019,21, 2639-2650

  •   Request permissions

    Computational QM/MM investigation of the adsorption of MTH active species in H-Y and H-ZSM-5

    S. A. F. Nastase, A. J. O’Malley, C. R. A. Catlow and A. J. Logsdail, Phys. Chem. Chem. Phys., 2019, 21, 2639
    DOI: 10.1039/C8CP06736H

Search articles by author

Spotlight

Advertisements