Effect of temperature on the conformation and functionality of poly(N-isopropylacrylamide) (PNIPAM)-grafted nanocellulose hydrogels

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dc.contributor.authorRaghuwanshi, VSen_AU
dc.contributor.authorMendoza, DJen_AU
dc.contributor.authorBrowne, Cen_AU
dc.contributor.authorAyurini, Men_AU
dc.contributor.authorGervinskas, Gen_AU
dc.contributor.authorHooper, JFen_AU
dc.contributor.authorMata, JPen_AU
dc.contributor.authorWu, CMen_AU
dc.contributor.authorSimon, GPen_AU
dc.contributor.authorGarnier, Gen_AU
dc.date.accessioned2024-01-11T21:28:49Zen_AU
dc.date.available2024-01-11T21:28:49Zen_AU
dc.date.issued2023-12-15en_AU
dc.date.statistics2023-11-21en_AU
dc.description.abstractHypothesis Poly(N-isopropylacrylamide) [PNIPAM]-grafted cellulose nanofibers (CNFs) are new thermo-responsive hydrogels which can be used for a wide range of applications. Currently, there is no clear understanding of the precise mechanism by which CNFs and PNIPAM interact together. Here, we hypothesize that the physical crosslinking of grafted PNIPAM on CNF inhibits the free movement of individual CNF, which increases the gel strength while sustaining its thermo-responsive properties. Experiments The thermo-responsive behaviour of PNIPAM-grafted CNFs (PNIPAM-g-CNFs), synthesized via silver-catalyzed decarboxylative radical polymerization, and PNIPAM-blended CNFs (PNIPAM-b-CNFs) was studied. Small angle neutron scattering (SANS) combined with Ultra-SANS (USANS) revealed the nano to microscale conformation changes of these polymer hybrids as a function of temperature. The effect of temperature on the optical and viscoelastic properties of hydrogels was also investigated. Findings Grafting PNIPAM from CNFs shifted the lower critical solution temperature (LCST) from 32 °C to 36 °C. Below LCST, the PNIPAM chains in PNIPAM-g-CNF sustain an open conformation and poor interaction with CNF, and exhibit water-like behaviour. At and above LCST, the PNIPAM chains change conformation to entangle and aggregate nearby CNFs. Large voids are formed in solution between the aggregated PNIPAM-CNF walls. In comparison, PNIPAM-b-CNF sustains liquid-like behaviour below LCST. At and above LCST, the blended PNIPAM phase separates from CNF to form large aggregates which do not affect CNF network and thus PNIPAM-b-CNF demonstrates low viscosity. Understanding of temperature-dependent conformation of PNIPAM-g-CNFs engineer thermo-responsive hydrogels for biomedical and functional applications. © 2023 The Author(s). Published by Elsevier Inc. This is an open access article under the CC BY-NC-ND license.en_AU
dc.description.sponsorshipThe authors would like to acknowledge the Australian Research Council (ARC) - Industrial Transformation Hub Grant IH170100020. The authors thank the Australian Nuclear Science and Technology Organisation (ANSTO) for the beamtime (Proposal ID:P14196). The authors acknowledge assistance and support of A/Prof. Georg Ramm as well as the use of instruments at the Monash Ramaciotti Centre for Cryo-Electron Microscopy, a Node of Microscopy Australia. The authors also acknowledge the use of the instruments and scientific and technical assistance of Dr. Tim Williams at the Monash Centre for Electron Microscopy, a Node of Microscopy Australia. This research used FEI Tecnai G2 F20 S-TWIN FEGTEM funded by ARC Grant LE110100223.en_AU
dc.identifier.citationRaghuwanshi, V. S., Mendoza, D. J., Browne, C., Ayurini, M., Gervinskas, G., Hooper, J. F., Mata, J. P., Wu, C.-M., Simon, G. P., & Garnier, G. (2023). Effect of temperature on the conformation and functionality of poly (N-isopropylacrylamide) (PNIPAM)-grafted nanocellulose hydrogels. Journal of Colloid and Interface Science, 652, Part B, 1609-1619. doi:10.1016/j.jcis.2023.08.152en_AU
dc.identifier.issn0021-9797en_AU
dc.identifier.issueBen_AU
dc.identifier.journaltitleJournal of Colloid and Interface Scienceen_AU
dc.identifier.pagination1609-1619en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15327en_AU
dc.identifier.volume652en_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.relation.urihttps://doi.org/10.1016/j.jcis.2023.08.152en_AU
dc.subjectGraftsen_AU
dc.subjectCelluloseen_AU
dc.subjectNanofibersen_AU
dc.subjectSmall angle scatteringen_AU
dc.subjectRheologyen_AU
dc.subjectHydrogelsen_AU
dc.titleEffect of temperature on the conformation and functionality of poly(N-isopropylacrylamide) (PNIPAM)-grafted nanocellulose hydrogelsen_AU
dc.typeJournal Articleen_AU
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