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

Padovan, Daniele, Botti, Luca and Hammond, Ceri ORCID: https://orcid.org/0000-0002-9168-7674 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Status:	Unpublished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:	22 Apr 2024 17:17
URI:	https://orca.cardiff.ac.uk/id/eprint/112523

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