A spectroscopic paradox: the interaction of methanol with ZSM-5 at room temperature

Zachariou, A., Hawkins, A. P. , Howe, R. F., Barrow, N., Bradley, J., Collier, P., Lennon, D. and Parker, S. F. (2021) A spectroscopic paradox: the interaction of methanol with ZSM-5 at room temperature. Topics in Catalysis, 64(9-12), pp. 672-684. (doi: 10.1007/s11244-021-01462-9)

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Abstract

The adsorption of methanol in HZSM-5 at low temperatures has long been regarded as an associative process involving hydrogen bonding to the acidic zeolite hydroxyl groups. Recent studies employing inelastic neutron scattering spectroscopy (INS) have reported that complete dissociation to methoxylate the zeolite occurs at 298 K, and infrared evidence for a partial dissociation at 298 K has also been described. Here we investigate the apparent contradictions between different techniques, using a combination of INS, infrared spectroscopy and solid-state NMR spectroscopy, including isotopic substitution experiments. Different possible explanations are proposed and considered; we conclude that at room temperature methanol is very largely associatively adsorbed, although the presence of some small extent (>1%) of methoxylation cannot be ruled out.

Item Type:Articles
Additional Information:Johnson Matthey plc. is thanked for supplying the ZSM-5 zeolite and for financial support through the provision of industrial CASE studentships in partnership with the EPSRC (APH (EP/P510506/1, AZ (EP/N509176/1)). Experiments at the ISIS Neutron and Muon Source were made possible by beam time allocations from the Science and Technologies Facilities Council.35-38 The resources and support provided by the UK Catalysis Hub via membership of the UK Catalysis Hub consortium and funded by EPSRC grants EP/R026815/1 and EP/R026939/1 are gratefully acknowledged.
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Parker, Dr Stewart and Zachariou, Andrea and Lennon, Professor David and Hawkins, Alexander
Authors: Zachariou, A., Hawkins, A. P., Howe, R. F., Barrow, N., Bradley, J., Collier, P., Lennon, D., and Parker, S. F.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Topics in Catalysis
Publisher:Springer
ISSN:1022-5528
ISSN (Online):1572-9028
Published Online:29 July 2021
Copyright Holders:Copyright © 2021 The Authors
First Published:First published in Topics in Catalysis 64(9-12): 672-684
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
172921EPSRC 2016 Industrial Case Award (iCASE) - JaguarMiles PadgettEngineering and Physical Sciences Research Council (EPSRC)16000061 - EP/P510506/1Research and Innovation Services
172233Anderson ICASE 2015 (Selex)Heather LambieEngineering and Physical Sciences Research Council (EPSRC)IND CASE EP/N509176/1S&E - Academic & Student Administration