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 |
Preview |
PDF
- Published Version
Download (1MB) | Preview |
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: | 05 May 2023 23:37 |
URI: | https://orca.cardiff.ac.uk/id/eprint/135089 |
Citation Data
Cited 14 times in Scopus. View in Scopus. Powered By Scopus® Data
Actions (repository staff only)
Edit Item |