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CNC_XG_TS_hydrogels_ChemRxiv.pdf (4.22 MB)

Bioinspired Thermo-Responsive Xyloglucan-Cellulose Nanocrystal Hydrogels

submitted on 04.08.2020, 12:38 and posted on 05.08.2020, 07:54 by Malika Talantikite, Taylor C. Stimpson, Antoine Gourlay, Sophie Le-Gall, Céline Moreau, Emily D. Cranston, Jose Moran-Mirabal, Bernard Cathala
Thermo-responsive hydrogels present unique properties, such as tunable mechanical performance or changes in volume, which make them attractive for applications including wound healing dressings, drug delivery vehicles, and implants, among others. This work reports the implementation of bio-based thermo-responsive hydrogels comprised of xyloglucan (XG) and cellulose nanocrystals (CNCs). Thermo-responsive properties were obtained by enzymatic degalactosylation of tamarind seed XG (DG-XG), which reduced the galactose residue content by ~50%, and imparted a reversible thermal transition. XG with comparable molar mass to DG-XG was achieved by ultrasonication treatment (XGu) for direct comparison of behavior. The hydrogels were prepared by simple mixing of DG-XG or XGu with CNCs in water. Phase diagrams were established to identify the ratios of DG-XG or XGu to CNCs (from 1:300 to 20:1 by mass) that yielded a viscous liquid, a phase separated mixture, a simple gel, or a thermo-responsive gel. Gelation occurred at a DG-XG or XGu to CNC ratio higher than that needed for the full surface coverage of CNCs, and required relatively high overall concentrations of both components (tested concentrations up to 20 g/L XG and 30 g/L CNCs). This is likely a result of the increase in effective hydrodynamic volume of CNCs due to the formation of XG-CNC complexes. Investigation of the adsorption behavior indicated that DG-XG formed a more rigid layer on CNCs compared to XGu. Rheological properties of the hydrogels were characterized and a reversible thermal transition was found for DG-XG/CNC gels at 35°C, where the mechanical properties of the gel could be tuned by adjusting the CNC content


Labex Serenade program (no. ANR-11-LABX-0064) funded by the “Investissements d'Avenir” programme of the French National Research Agency (ANR) through the A*MIDEX project (no. ANR-11-IDEX-0001-02)

HOBIT program financed by the Pays de la Loire region. T

T.C.S is the recipient of a Queen Elizabeth II Ontario Graduate Scholarship and was partially supported through a Mitacs Globalink Graduate Fellowship. J

J.M.M. and E.D.C. are recipients of Early Researcher awards from the Ontario Ministry of Research and Innovation.

J.M.M. is the Tier 2 Canada Research Chair in Micro and Nanostructured Materials


Email Address of Submitting Author


UR1268 BIA, INRAE, Nantes



ORCID For Submitting Author


Declaration of Conflict of Interest

no conflict of interest

Version Notes

preprint version 1