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

Research output: Contribution to journalArticlepeer-review

48 Citations (Scopus)
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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 languageEnglish
Pages (from-to)6564-6570
Number of pages7
JournalACS Catalysis
Volume9
Issue number7
Early online date17 Jun 2019
DOIs
Publication statusPublished - 5 Jul 2019

Bibliographical 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).

Keywords

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

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