Identification of active and spectator Sn sites in Sn-β following solid-state stannation, and consequences for Lewis acid catalysis

Hammond, Ceri ORCID: https://orcid.org/0000-0002-9168-7674, Padovan, Daniele, Al-Nayili, Abbas, Wells, Peter P., Gibson, Emma K. and Dimitratos, Nikolaos ORCID: https://orcid.org/0000-0002-6620-4335 2015. Identification of active and spectator Sn sites in Sn-β following solid-state stannation, and consequences for Lewis acid catalysis. ChemCatChem 7 (20) , pp. 3322-3331. 10.1002/cctc.201500545

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Abstract

Lewis acidic zeolites are rapidly emerging liquid-phase Lewis acid catalysts. Nevertheless, their inefficient synthesis procedure currently prohibits greater utilization and exploitation of these promising materials. Herein, we demonstrate that SnIV-containing zeolite beta can readily be prepared both selectively and extremely rapidly by solid-state incorporation (SSI) method. Through a combination of spectroscopic (XRD, UV/Vis, X-ray absorption, magic-angle spinning NMR, and diffuse reflectance infrared Fourier transform spectroscopy) studies, we unambiguously demonstrate that site-isolated, isomorphously substituted SnIV sites dominate the Sn population up to a loading of 5 wt % Sn. These sites are identical to those found in conventionally prepared Sn-beta, and result in our SSI material exhibiting identical levels of intrinsic activity (that is, turnover frequency) despite the threefold increase in Sn loading, and the extremely rapid and benign nature of our preparation methodology. We also identify the presence of spectator sites, in the form of SnIV oligomers, at higher levels of Sn loading. The consequences of this mixed population with regards to catalysis (Meerwein–Pondorf–Verley reaction and glucose isomerization) are also identified.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry
Subjects:	Q Science > QD Chemistry
Publisher:	Wiley
ISSN:	1867-3880
Funders:	EPSRC
Date of First Compliant Deposit:	30 March 2016
Date of Acceptance:	8 June 2015
Last Modified:	13 May 2023 18:36
URI:	https://orca.cardiff.ac.uk/id/eprint/77075

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