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Solvent‐activated hafnium‐containing zeolites enable selective and continuous glucose–fructose isomerisation

Botti, Luca, Kondrat, Simon A., Navar, Ricardo, Padovan, Daniele, Martinez-Espin, Juan S., Meier, Sebastian and Hammond, Ceri 2020. Solvent‐activated hafnium‐containing zeolites enable selective and continuous glucose–fructose isomerisation. Angewandte Chemie International Edition 59 (45) , pp. 20017-20023. 10.1002/anie.202006718

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Abstract

The isomerisation of glucose to fructose is a critical step towards manufacturing petroleum‐free chemicals from lignocellulosic biomass. Herein we show that Hf‐containing zeolites are unique catalysts for this reaction, enabling true thermodynamic equilibrium to be achieved in a single step during intensified continuous operation, which no chemical or biological catalyst has yet been able to achieve. Unprecedented single‐pass yields of 58 % are observed at a fructose selectivity of 94 %, and continuous operation for over 100 hours is demonstrated. The unexpected performance of the catalyst is realised following a period of activation within the reactor, during which time interaction with the solvent generates a state of activity that is absent in the synthesised catalyst. Mechanistic studies by X‐ray absorption spectroscopy, chemisorption FTIR, operando UV/Vis and 1H–13C HSQC NMR spectroscopy indicate that activity arises from isolated HfIV atoms with monofunctional acidic properties.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Wiley
ISSN: 1433-7851
Date of First Compliant Deposit: 24 September 2020
Date of Acceptance: 20 July 2020
Last Modified: 12 Nov 2020 12:43
URI: http://orca.cardiff.ac.uk/id/eprint/135089

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