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

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journal contribution
posted on 22.01.2021, 13:46 by Luca Botti, Simon KondratSimon Kondrat, Ricardo Navar, Daniele Padovan, Juan S. Martinez-Espin, Sebastian MeierSebastian Meier, Ceri Hammond
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.

Funding

Royal Society UF140207

Royal Society RGF/EA/180314

Consejo Nacional de Ciencia y Tecnología. Grant Number: 472256

Royal Society URF\R\201003

History

School

  • Science

Department

  • Chemistry

Published in

Angewandte Chemie International Edition

Volume

59

Issue

45

Pages

20017 - 20023

Publisher

Wiley

Version

VoR (Version of Record)

Rights holder

© The Authors

Publisher statement

This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

Acceptance date

20/07/2020

Publication date

2020-08-31

ISSN

0044-8249

eISSN

1521-3773

Language

en

Depositor

Deposit date: 22 January 2021