Differentiating the role of organic additives to assemble open framework aluminosilicates using INS spectroscopy

Antony Nearchou, Jeff Armstrong, Keith Butler, Paul Raithby, Asel Sartbaeva

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Abstract

Presently, there is little clarity concerning how organic additives control structure formation in the synthesis of zeolite catalysts. Such ambiguity is a major obstacle towards synthesis design of new bespoke zeolites with intended applications. Herein, we have applied inelastic neutron scattering (INS) spectroscopy to experimentally probe the nature of organic-framework interactions, which are crucial in understanding structure direction. With this technique we have studied the dynamics of 18-crown-6 ether, which can be used as an additive to direct the formation of four zeolites: Na-X, EMC-2, RHO and ZK-5. We observed significant softening of the 18-crown-6 ether molecule's dynamics upon occlusion within a zeolite host, with a strong influence on both the circular and radial vibrational modes. Furthermore, there is a strong correlation between the size/geometry of the zeolite framework cages and perturbations in the dynamics of the 18C6 oxyethylene chain. We propose that the approach used herein can be used to study other zeolites, and hence gain a more comprehensive view of organic-framework interactions.

Original languageEnglish
Pages (from-to)14177-14186
Number of pages10
JournalPhysical Chemistry Chemical Physics
Volume22
Issue number25
DOIs
Publication statusPublished - 11 Jun 2020

Bibliographical note

Funding Information:
A. S. thanks the Royal Society for funding. Both A. N. and P. R. R. thank the EPSRC for funding (EP/K004956/1). The INS spectra herein were collected on the TOSCA instrument at ISIS Neutron and Muon Source, Didcot, UK. We thank the STFC for accepting our research proposal.

Publisher Copyright:
© 2020 the Owner Societies.

Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.

Keywords

  • Zeolite
  • INS spectroscopy
  • aluminosilicate
  • hydrothermal synthesis
  • Neutron scattering
  • vibrational spectroscopy
  • spectroscopy
  • template
  • organic additive

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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