Designed Synthesis Of Sta-30: A Small-Pore Zeolite Catalyst With Topology Type Swy

CHEMISTRY OF MATERIALS(2021)

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摘要
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, P6(3)/ mmc, a = 12.9922(9) angstrom, c = 29.9624(12) angstrom) with solid acidity shown by solid-state H-1 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 Al-27 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 cm(3) g(-1). In the copper-loaded form, it is an active catalyst for the SCR of NO by ammonia.
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关键词
zeolite,catalyst,topology type swy,small-pore
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