Facile, Room-Temperature 17 O Enrichment of Zeolite Frameworks Revealed by Solid-State NMR Spectroscopy

A new approach for room-temperature O enrichment of zeolites reveals a surprisingly dynamic and labile framework, where rapid and reversible bond breaking takes place. O NMR spectroscopy shows that although O sites in both framework Si-O-Al and Si-O-Si linkages are enriched simply on exposure to H O...

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Veröffentlicht in:Journal of the American Chemical Society 2020-01, Vol.142 (2), p.900-906
Hauptverfasser: Pugh, Suzi M, Wright, Paul A, Law, David J, Thompson, Nicholas, Ashbrook, Sharon E
Format: Artikel
Sprache:eng
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Zusammenfassung:A new approach for room-temperature O enrichment of zeolites reveals a surprisingly dynamic and labile framework, where rapid and reversible bond breaking takes place. O NMR spectroscopy shows that although O sites in both framework Si-O-Al and Si-O-Si linkages are enriched simply on exposure to H O(l), the enrichment of Si-O-Al species is more rapid, with a more uniform framework enrichment observed at longer durations. We demonstrate that this unexpected enrichment can be observed for two different framework topologies and for Na-exchanged (i.e., nonacidic) zeolites, as well as their protonic forms, confirming that the Brønsted acid proton is not necessary for isotopic exchange into the framework. This work not only offers new opportunities for structural characterization of these chemically and industrially important materials using NMR spectroscopy but suggests that further investigation of the rate and position of enrichment in zeolite frameworks could provide new insight into their chemical reactivity and their stability in aqueous-based applications such as ion exchange and catalysis.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.9b10528