Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy

Ivalina B. Minova; Santhosh K. Matam; Alex Greenaway; C. Richard A.  Catlow; Mark D. Frogley; Gianfelice Cinque; Paul A. Wright; Russell F. Howe

doi:10.1021/acscatal.9b01820

Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy

Ivalina B. Minova, Santhosh K. Matam, Alex Greenaway, C. Richard A. Catlow, Mark D. Frogley, Gianfelice Cinque, Paul A. Wright, Russell F. Howe^* (Corresponding Author)

^*Corresponding author for this work

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Abstract

Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapour is contacted with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerise and cyclise to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocarbon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. The technique observes these events in real time.

Original language	English
Pages (from-to)	6564-6570
Number of pages	7
Journal	ACS Catalysis
Volume	9
Issue number	7
Early online date	17 Jun 2019
DOIs	https://doi.org/10.1021/acscatal.9b01820
Publication status	Published - 5 Jul 2019

Keywords

synchrotron infrared microspectroscopy
ZSM-5
methanol-to-hydrocarbons
hydrocarbon pool
carbon-carbon bond formation
micro-FTIR

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.9b01820.
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Russell Howe
- Chemistry (Research Theme)
- School of Natural & Computing Sciences, Chemistry - Chair of Chemistry
Person: Academic

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Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy. / Minova, Ivalina B.; Matam, Santhosh K.; Greenaway, Alex; Catlow, C. Richard A. ; Frogley, Mark D.; Cinque, Gianfelice; Wright, Paul A.; Howe, Russell F. (Corresponding Author).

In: ACS Catalysis, Vol. 9, No. 7, 05.07.2019, p. 6564-6570.

Research output: Contribution to journal › Article › peer-review

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title = "Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy",

abstract = "Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapour is contacted with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerise and cyclise to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocarbon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. The technique observes these events in real time.",

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note = "IBM and PAW would like to thank the EPSRC and CRITICAT Centre for Doctoral Training for Financial Support [PhD studentship to IBM, and supplementary equipment grant EP/L016419/1]. The UK Catalysis Hub is thanked for resources and support provided via membership of the UK Catalysis Hub Consortium and funded by EPSRC (grants EP/I038748/1, EP/I019693/1, EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1 and EP/M013219/1). We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM13725-1, SM16257-1, SM18680-1, SM20906-1).",

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AU - Frogley, Mark D.

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N1 - IBM and PAW would like to thank the EPSRC and CRITICAT Centre for Doctoral Training for Financial Support [PhD studentship to IBM, and supplementary equipment grant EP/L016419/1]. The UK Catalysis Hub is thanked for resources and support provided via membership of the UK Catalysis Hub Consortium and funded by EPSRC (grants EP/I038748/1, EP/I019693/1, EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1 and EP/M013219/1). We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM13725-1, SM16257-1, SM18680-1, SM20906-1).

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Elementary Steps in the Formation of Hydrocarbons from Surface Methoxy Groups in HZSM-5 Seen by Synchrotron Infrared Microspectroscopy

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Keywords

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Russell Howe

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