Thermoresponsive polysaccharides with tunable thermoresponsive properties via functionalisation with alkylamide groups

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dc.contributor.authorOtto, S.
dc.contributor.authorMarina, P.F.
dc.contributor.authorZhou, F.
dc.contributor.authorBlencowe, A.
dc.date.issued2021
dc.description.abstractPolysaccharides have been used widely in many industries, from food technology and mining to cosmetics and biomedical applications. Over recent years there has been growing interest in the development of responsive polysaccharides with unique and switchable properties, particularly systems that display lower-critical solution temperatures (LCSTs). Therefore, in this study we aimed to investigate a novel strategy that would allow the conversion of non-responsive polysaccharides into thermoresponsive polysaccharides with tuneable LCSTs. Through the functionalisation of dextran with alkylamide groups (isopropyl amide, diethyl amide, piperidinyl and diisobutyl amide) using a carbodiimide coupling approach in conjunction with amic acid derivatives, we prepared a library of novel dextrans with various degrees of substitution (DS), which were characterised via nuclear magnetic resonance (NMR) spectroscopy and gel permeation chromatography (GPC). The alkylamidefunctionalised dextrans were found to have good solubility in aqueous solutions, with the exception of those having a high DS of large hydrophobic substituents. Determination of the thermoresponsive characteristics of the polymer solutions via UV–vis spectroscopy revealed that the LCST of the alkylamide-functionalised dextrans was highly dependent on the type of alkylamide group and the DS and could be tuned over a large range (5–35 ◦C). Above the LCST, all of the thermoresponsive alkylamide-functionalised dextrans formed colloidal dispersions with particles sizes ranging from 400 -600 nm, as determined by dynamic light scattering (DLS). In addition, the polymers were found to exhibit a fast and reversible phase transition in solution with narrow hysteresis (~ 1–5 ◦C). Finally, the injectability and biocompatibility of the novel thermoresponsive dextrans was confirmed in vivo via subcutaneous and intracranial ventricle injections, with no local or systemic toxicity noted over a 14 d period. Overall, the alkylamide-functionalised dextrans display interesting thermoresponsive properties and trends that may make them useful in biomedical applications, such as drug-delivery.
dc.description.statementofresponsibilitySarah Otto, Paula Facal Marina, Fiona Zhou, Anton Blencowe
dc.identifier.citationCarbohydrate Polymers, 2021; 254:1172801-117280-12
dc.identifier.doi10.1016/j.carbpol.2020.117280
dc.identifier.issn0144-8617
dc.identifier.issn0144-8617
dc.identifier.orcidZhou, F. [0000-0003-3113-1671]
dc.identifier.urihttps://hdl.handle.net/2440/146434
dc.language.isoen
dc.publisherElsevier
dc.rights© 2020 Elsevier Ltd. All rights reserved.
dc.source.urihttps://doi.org/10.1016/j.carbpol.2020.117280
dc.subjectThermoresponsive; Polysaccharides; Alkylamides; Dextran; Lower-critical solution temperature
dc.subject.meshAnimals
dc.subject.meshMice, Inbred C57BL
dc.subject.meshMice
dc.subject.meshAmides
dc.subject.meshDextrans
dc.subject.meshPolysaccharides
dc.subject.meshBiocompatible Materials
dc.subject.meshChromatography, Gel
dc.subject.meshSpectrophotometry
dc.subject.meshNuclear Magnetic Resonance, Biomolecular
dc.subject.meshMaterials Testing
dc.subject.meshTemperature
dc.subject.meshMolecular Structure
dc.subject.meshAlkylation
dc.subject.meshMolecular Weight
dc.subject.meshParticle Size
dc.subject.meshPhase Transition
dc.subject.meshDynamic Light Scattering
dc.titleThermoresponsive polysaccharides with tunable thermoresponsive properties via functionalisation with alkylamide groups
dc.typeJournal article
pubs.publication-statusPublished

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