Modulating the isotopic hydrogen-deuterium exchange in functionalized nanocellulose to optimize SANS contrast

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dc.contributor.authorRaghuwanshi, VSen_AU
dc.contributor.authorMendoza, DJen_AU
dc.contributor.authorMata, JPen_AU
dc.contributor.authorGarnier, GFGen_AU
dc.date.accessioned2024-10-15T04:42:24Zen_AU
dc.date.available2024-10-15T04:42:24Zen_AU
dc.date.issued2024-12en_AU
dc.date.statistics2024-08-23en_AU
dc.description.abstractContrast matching by isotopic exchange in cellulose allows visualizing functional groups, biomolecules, polymers and nanoparticles embedded in cellulosic composites. This isotopic exchange varies the scattering length density of cellulose to match its contrast with the background network. Here, contrast matching of microcrystalline-cellulose (MCC) and the functionalized nanocellulose-fiber (CNF) and cellulose nanocrystals (CNC) are elucidated by small angle neutron scattering (SANS). Results show no isotopic exchange occurs for the CNF surface functionalized with carboxyl nor for the CNC-High with a high sulfate groups concentration. Both CNC-Low, with low sulfate groups, and MCC exchange 1H with 1D in D2O. This is due to the high exchange probability of the labile C6 position primary -OH group. The structure of thermo-responsive poly-N-isopropylacrylamide (PNIPAM) chains grafted onto CNF (PNIPAM-grafted-CNF) was extracted by CNF contrast matching near the lower critical solution temperature. Contrast matching eradicates the CNF scattering to retain only the scattering from the grafted-PNIPAM chains. The coil to globule thermo-transition of PNIPAM was revealed by the power law variation from q−1.3 to q−4 in SANS. Isotopic exchange in functionalized cellulosic materials reveals the nano- and micro-scale structure of its individual components. This improved visualization by contrast matching can be extended to carbohydrate polymers to engineer biopharmaceutical and food applications. © 2024 The Authors. Published by Elsevier Ltd. - Open Access CC BY 4.0en_AU
dc.description.sponsorshipWe acknowledge funding from the Australian Research Council (ARC) - Industrial Transformation Hub Grant IH130100016. Thanks to the Australian Nuclear Science and Technology Organisation (ANSTO) for the beamtime (Proposal ID: DB 17373). Authors thank to Dr. Christine Browne and Asso/Prof. Warren Batchelor for assistance during beamtime.en_AU
dc.identifier.articlenumber122591en_AU
dc.identifier.citationRaghuwanshi, V. S., Mendoza, D. J., Mata, J., & Garnier, G. (2024). Modulating the isotopic hydrogen-deuterium exchange in functionalized nanocellulose to optimize SANS contrast. Carbohydrate Polymers, 345, 122591. doi:10.1016/j.carbpol.2024.122591en_AU
dc.identifier.issn0144-8617en_AU
dc.identifier.journaltitleCarbohydrate Polymersen_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15745en_AU
dc.identifier.volume345en_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.relation.urihttps://doi.org/10.1016/j.carbpol.2024.122591en_AU
dc.subjectContrast Mediaen_AU
dc.subjectSmall angle scatteringen_AU
dc.subjectDeuteriumen_AU
dc.subjectIsotopesen_AU
dc.subjectCelluloseen_AU
dc.subjectNanocrystalsen_AU
dc.subjectCarboxylaseen_AU
dc.titleModulating the isotopic hydrogen-deuterium exchange in functionalized nanocellulose to optimize SANS contrasten_AU
dc.typeJournal Articleen_AU
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