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

Ruxandra Georgiana Chitac, Jonathan Bradley, Nicholas McNamara, Alvaro Mayoral, Alessandro Turrina, Paul Anthony Wright

Research output: Contribution to journalArticlepeer-review

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 (K3H6Al9Si72O144P63/mmca = 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.

Original languageEnglish
Number of pages15
JournalChemistry of Materials
VolumeArticles ASAP
Early online date18 Jun 2021
DOIs
Publication statusE-pub ahead of print - 18 Jun 2021

Keywords

  • Genetics
  • Zeolites
  • Chemical structure
  • Cations
  • Materials

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