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Active site hydration governs the stability of Sn-Beta during continuous glucose conversion

Padovan, Daniele, Botti, Luca and Hammond, Ceri 2018. Active site hydration governs the stability of Sn-Beta during continuous glucose conversion. ACS Catalysis 10.1021/acscatal.8b01759

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Abstract

The stability of Sn-Beta for the continuous upgrading of hexoses is improved dramatically upon the addition of small amounts of water to the methanol/sugar reaction feed, despite water itself being an unfavourable solvent. Herein, the molecular level origin of this effect is investigated. Spectroscopic studies of the catalytic materials pre-, post- and during operation, with in situ UV-Vis, 119Sn CPMG MAS NMR, DRIFTS-MS, TGA, TPD/O-MS and porosimetry, are coupled to additional kinetic studies, to generate detailed structure-activity-lifetime relationships. In doing so, we find that the addition of water influences two particular processes – fouling and active site modification. However, mitigating the second is the most crucial role of water. Indeed, in the absence of water, the loss of Sn-OH and Si-OH sites occurs. Notably, these changes in active site hydration correlate to deactivation and reac-tivation of the system. The consequences of these findings, both for mechanistic understanding of the system in addition to the design of alternative regeneration methods, are also discussed.

Item Type: Article
Date Type: Published Online
Status: Unpublished
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: American Chemical Society
ISSN: 2155-5435
Funders: The Royal Society
Date of First Compliant Deposit: 18 June 2018
Date of Acceptance: 15 June 2018
Last Modified: 09 Jun 2020 01:27
URI: http://orca-mwe.cf.ac.uk/id/eprint/112523

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