Reactions of Dimethylether in Single Crystals of the Silicoaluminophosphate STA-7 Studied via Operando Synchrotron Infrared Microspectroscopy

Russell F. Howe*, Suwardiyanto, David J. Price, Maria Castro, Paul A. Wright, Alex Greenaway, Mark D. Frogley, Gianfelice Cinque

*Corresponding author for this work

Research output: Contribution to journalArticle

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Abstract

Abstract: Synchrotron infrared micro-spectroscopy has been applied to measure in situ the reaction of dimethylether in single crystals of the silicoaluminophosphate STA-7. The crystals are found to contain a uniform and homogeneous distribution of acidic hydroxyl groups. Dimethylether is hydrogen bonded to the hydroxyl groups at low temperatures, but evidence is found for dissociation to form surface methoxy groups above 473 K, and aromatic hydrocarbon pool species above 573 K. From time resolved infrared measurements coupled with MS analysis of evolved products it is concluded that alkene formation occurs via a direct mechanism from reaction of dimethylether with surface methoxy groups. Graphical Abstract: [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)1-14
Number of pages14
JournalTopics in Catalysis
Volume61
Issue number3-4
Early online date16 Jan 2018
DOIs
Publication statusPublished - Apr 2018

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Synchrotrons
Hydroxyl Radical
Single crystals
Infrared radiation
Aromatic Hydrocarbons
Aromatic hydrocarbons
Alkenes
Olefins
Hydrogen
Spectroscopy
Crystals
Temperature

Keywords

  • Dimethylether
  • Hydrocarbon pool
  • Infrared microspectroscopy
  • STA-7

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Reactions of Dimethylether in Single Crystals of the Silicoaluminophosphate STA-7 Studied via Operando Synchrotron Infrared Microspectroscopy. / Howe, Russell F.; Suwardiyanto; Price, David J.; Castro, Maria; Wright, Paul A.; Greenaway, Alex; Frogley, Mark D.; Cinque, Gianfelice.

In: Topics in Catalysis, Vol. 61, No. 3-4, 04.2018, p. 1-14.

Research output: Contribution to journalArticle

Howe, Russell F. ; Suwardiyanto ; Price, David J. ; Castro, Maria ; Wright, Paul A. ; Greenaway, Alex ; Frogley, Mark D. ; Cinque, Gianfelice. / Reactions of Dimethylether in Single Crystals of the Silicoaluminophosphate STA-7 Studied via Operando Synchrotron Infrared Microspectroscopy. In: Topics in Catalysis. 2018 ; Vol. 61, No. 3-4. pp. 1-14.
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abstract = "Abstract: Synchrotron infrared micro-spectroscopy has been applied to measure in situ the reaction of dimethylether in single crystals of the silicoaluminophosphate STA-7. The crystals are found to contain a uniform and homogeneous distribution of acidic hydroxyl groups. Dimethylether is hydrogen bonded to the hydroxyl groups at low temperatures, but evidence is found for dissociation to form surface methoxy groups above 473 K, and aromatic hydrocarbon pool species above 573 K. From time resolved infrared measurements coupled with MS analysis of evolved products it is concluded that alkene formation occurs via a direct mechanism from reaction of dimethylether with surface methoxy groups. Graphical Abstract: [Figure not available: see fulltext.]",
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note = "Open access via the Springer Compact Agreement. We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM11766-1 and SM13725-1). Financial support from the EPSRC Catalysis Hub (Suwardiyanto) and an Industrial CASE Award (EPSRC/BP Chemicals) (Price) are also acknowledged.",
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AU - Wright, Paul A.

AU - Greenaway, Alex

AU - Frogley, Mark D.

AU - Cinque, Gianfelice

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N2 - Abstract: Synchrotron infrared micro-spectroscopy has been applied to measure in situ the reaction of dimethylether in single crystals of the silicoaluminophosphate STA-7. The crystals are found to contain a uniform and homogeneous distribution of acidic hydroxyl groups. Dimethylether is hydrogen bonded to the hydroxyl groups at low temperatures, but evidence is found for dissociation to form surface methoxy groups above 473 K, and aromatic hydrocarbon pool species above 573 K. From time resolved infrared measurements coupled with MS analysis of evolved products it is concluded that alkene formation occurs via a direct mechanism from reaction of dimethylether with surface methoxy groups. Graphical Abstract: [Figure not available: see fulltext.]

AB - Abstract: Synchrotron infrared micro-spectroscopy has been applied to measure in situ the reaction of dimethylether in single crystals of the silicoaluminophosphate STA-7. The crystals are found to contain a uniform and homogeneous distribution of acidic hydroxyl groups. Dimethylether is hydrogen bonded to the hydroxyl groups at low temperatures, but evidence is found for dissociation to form surface methoxy groups above 473 K, and aromatic hydrocarbon pool species above 573 K. From time resolved infrared measurements coupled with MS analysis of evolved products it is concluded that alkene formation occurs via a direct mechanism from reaction of dimethylether with surface methoxy groups. Graphical Abstract: [Figure not available: see fulltext.]

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