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Modelling metal centres, acid sites and reaction mechanisms in microporous catalysts

O'Malley, AJ; Logsdail, AJ; Sokol, AA; Catlow, CR; (2016) Modelling metal centres, acid sites and reaction mechanisms in microporous catalysts. Faraday Discussions , 188 pp. 235-255. 10.1039/c6fd00010j. Green open access

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Abstract

We discuss the role of QM/MM (embedded cluster) computational techniques in catalytic science, in particular their application to microporous catalysis. We describe the methodologies employed and illustrate their utility by briefly summarising work on metal centres in zeolites. We then report a detailed investigation into the behaviour of methanol at acidic sites in zeolites H-ZSM-5 and H-Y in the context of the methanol-to-hydrocarbons/olefins process. Studying key initial steps of the reaction (the adsorption and subsequent methoxylation), we probe the effect of framework topology and Brønsted acid site location on the energetics of these initial processes. We find that although methoxylation is endothermic with respect to the adsorbed system (by 17-56 kJ mol(-1) depending on the location), there are intriguing correlations between the adsorption/reaction energies and the geometries of the adsorbed species, of particular significance being the coordination of methyl hydrogens. These observations emphasise the importance of adsorbate coordination with the framework in zeolite catalysed conversions, and how this may vary with framework topology and site location, particularly suited to investigation by QM/MM techniques.

Type: Article
Title: Modelling metal centres, acid sites and reaction mechanisms in microporous catalysts
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/c6fd00010j
Publisher version: http://dx.doi.org/10.1039/c6fd00010j
Language: English
Additional information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/1494188
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