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A multinuclear NMR study of six forms of AlPO-34 : structure and motional broadening

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Date
26/01/2017
Author
Dawson, Daniel M.
Griffin, John M.
Seymour, Valerie R.
Wheatley, Paul S.
Amri, Mahrez
Kurkiewicz, Teresa
Guillou, Nathalie
Wimperis, Stephen
Walton, Richard
Ashbrook, Sharon E.
Funder
EPSRC
The Leverhulme Trust
Grant ID
EP/M022501/1
F/00 268/BJ
Keywords
QD Chemistry
DAS
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Abstract
We report a study of the CHA-type aluminophosphate AlPO-34, prepared with six different structure-directing agents (SDAs): piperidine (pip), morpholine (mor), pyridine (pyr), 1,4,8,11-tetraazacyclotetradecane (cyclam), 1,3-dimethylimidazolium (dmim) chloride and 1-ethyl-3-methylimidazolium (emim) bromide. Using a combination of solid-state NMR spectroscopy, periodic density functional theory (DFT) calculations and synchrotron X-ray diffraction, we show that, even in crystallographically well-ordered materials such as AlPO-34 with dmim as the SDA, local disorder may be present. For such disordered structures, where it is challenging to use DFT to assign NMR spectra, we show that the 31P isotropic chemical shift can be predicted accurately using the mean P-O bond length and P-O-Al bond angle, in an extension of previous work. Variable-temperature 27Al NMR reveals the presence of microsecond-timescale dynamics in all forms of AlPO-34, with two different motional regimes observed, depending on whether structural H2O is also present. H2O is detected in AlPO-34 prepared with mor as the SDA, although this material was previously reported as anhydrous, suggesting that this form of AlPO-34 may be hygroscopic despite the presence of the SDAs within the pores.
Citation
Dawson , D M , Griffin , J M , Seymour , V R , Wheatley , P S , Amri , M , Kurkiewicz , T , Guillou , N , Wimperis , S , Walton , R & Ashbrook , S E 2017 , ' A multinuclear NMR study of six forms of AlPO-34 : structure and motional broadening ' , Journal of Physical Chemistry C , vol. 121 , no. 3 , pp. 1781-1793 . https://doi.org/10.1021/acs.jpcc.6b11908
Publication
Journal of Physical Chemistry C
Status
Peer reviewed
DOI
https://doi.org/10.1021/acs.jpcc.6b11908
ISSN
1932-7447
Type
Journal article
Rights
Copyright © 2017 American Chemical Society. This work has been made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at: https://doi.org/10.1021/acs.jpcc.6b11908
Description
SEA would like to thank the Leverhulme Trust (F/00 268/BJ) and EPSRC for computational support through the Collaborative Computational Project on NMR Crystallography (CCP-NC), via EP/M022501/1). SEA would also like to thank the Royal Society and Wolfson Foundation for a merit award. MA and RIW would like to acknowledge financial support from the EPSRC (EP/C516591), as would SW (GR/T23824). The research data (and/or materials) supporting this publication can be accessed at DOI: 10.17630/a6d6d27b-a8f0-46cb-8e6b-2c9a344e86b7.
Collections
  • University of St Andrews Research
URI
http://hdl.handle.net/10023/12420

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