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Designed synthesis of STA-30 : a small pore zeolite catalyst with topology type SWY

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Date
18/06/2021
Author
Chitac, Ruxandra Georgiana
Bradley, Jonathan
McNamara, Nicholas
Mayoral, Alvaro
Turrina, Alessandro
Wright, Paul Anthony
Funder
EPSRC
The Royal Society
Grant ID
EP/S016201/1
INF\R2\192052
Keywords
Genetics
Zeolites
Chemical structure
Cations
Materials
QD Chemistry
DAS
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Abstract
Small-pore aluminosilicate zeolites are attractive targets for synthesis because of their activity as catalysts in important reactions, including ammonia-mediated selective catalytic reduction (SCR) of NOx in auto-exhaust emissions. Such a zeolite with SWY framework type, previously observed as a silicoaluminophosphate, has been prepared with high crystallinity via designed syntheses employing organic 1,8-(1,4-diazabicyclo[2.2.2]octane)octyl (diDABCO-C8) and K+ cations as templates. STA-30 (St Andrews microporous material 30) is an ABC-6 structure in the erionite-offretite family of zeolites that exhibits the 12-layer stacking sequence AABAABAACAAC. The framework, which can be prepared with a controllable Si/Al ratio, possesses columns of alternating d6r units and can cages, of which the latter are oriented to give an inter-column pore space comprising gme cages and swy cages connected via 8Rs. DiDABCO-C8 cations fill the swy cages of as-prepared STA-30, while K+ cations display high occupancy in the can cages. Removal of the template by calcination, followed by ammonium ion exchange of K+ cations residing outside the can cages and subsequent deammoniation, gives a highly crystalline zeolite (K3H6Al9Si72O144, P63/mmc, a = 12.9922(9) Å, c = 29.9624(12) Å) with solid acidity shown by solid-state 1H MAS NMR. Upon hydration, a portion of the Al adopts octahedral geometry, as demonstrated by two sharp resonances at −2.0 and −3.1 ppm in the 27Al MAS NMR. These octahedral species can be converted back to tetrahedral Al by ammonium exchange and are interpreted as distinct hydrated framework Al sites. The activated K,H-STA-30 is a small-pore solid acid with a three-dimensionally connected micropore volume of 0.31 cm3 g–1. In the copper-loaded form, it is an active catalyst for the SCR of NO by ammonia.
Citation
Chitac , R G , Bradley , J , McNamara , N , Mayoral , A , Turrina , A & Wright , P A 2021 , ' Designed synthesis of STA-30 : a small pore zeolite catalyst with topology type SWY ' , Chemistry of Materials , vol. Articles ASAP . https://doi.org/10.1021/acs.chemmater.1c01329
Publication
Chemistry of Materials
Status
Peer reviewed
DOI
https://doi.org/10.1021/acs.chemmater.1c01329
ISSN
0897-4756
Type
Journal article
Rights
Copyright © 2021 American Chemical Society. This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted 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.chemmater.1c01329
Description
R.G.C. thanks the University of St Andrews and Johnson Matthey for funding. P.A.W. thanks the EPSRC (Designed Synthesis of Zeolites: EP/S016201/1) and the Royal Society (Industry Fellowship INF\R2\192052) for support. A.M. acknowledges the Spanish Ministry of Science and Innovation through the Ramon y Cajal programme (RYC2018-024561-I), the Regional government of Aragon (DGA E13_20R), and to the National Natural Science Foundation of China (NFSC-21850410448; NSFC-21835002).
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  • University of St Andrews Research
URI
http://hdl.handle.net/10023/25545

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