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Solvent‐Activated Hafnium‐Containing Zeolites Enable Selective and Continuous Glucose–Fructose Isomerisation
Author(s) -
Botti Luca,
Kondrat Simon A.,
Navar Ricardo,
Padovan Daniele,
MartinezEspin Juan S.,
Meier Sebastian,
Hammond Ceri
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202006718
Subject(s) - catalysis , isomerization , chemistry , selectivity , zeolite , solvent , fructose , fourier transform infrared spectroscopy , inorganic chemistry , chemisorption , organic chemistry , chemical engineering , engineering
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 1 H– 13 C HSQC NMR spectroscopy indicate that activity arises from isolated Hf IV atoms with monofunctional acidic properties.