Solvent-activated hafnium-containing zeolites enable selective and continuous glucose–fructose isomerisation
journal contributionposted on 22.01.2021, 13:46 by Luca Botti, Simon Kondrat, Ricardo Navar, Daniele Padovan, Juan S. Martinez-Espin, Sebastian 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.
Royal Society UF140207
Royal Society RGF/EA/180314
Consejo Nacional de Ciencia y Tecnología. Grant Number: 472256
Royal Society URF\R\201003