Structural evolution of photocrosslinked silk fibroin and silk fibroin-based hybrid hydrogels: a small angle and ultra-small angle scattering investigation

dc.contributor.authorWhittaker, JLen_AU
dc.contributor.authorBalu, Ren_AU
dc.contributor.authorKnott, RBen_AU
dc.contributor.authorde Campo, Len_AU
dc.contributor.authorMata, JPen_AU
dc.contributor.authorRehm, Cen_AU
dc.contributor.authorHill, AJen_AU
dc.contributor.authorDutta, NKen_AU
dc.contributor.authorChoudhury, NRen_AU
dc.date.accessioned2023-11-16T21:34:10Zen_AU
dc.date.available2023-11-16T21:34:10Zen_AU
dc.date.issued2018-07-15en_AU
dc.date.statistics2023-11-14en_AU
dc.descriptionPreprint version attached.en_AU
dc.description.abstractRegenerated Bombyx mori silk fibroin (RSF) is a widely recognized protein for biomedical applications; however, its hierarchical gel structure is poorly understood. In this paper, the hierarchical structure of photocrosslinked RSF and RSF-based hybrid hydrogel systems: (i) RSF/Rec1-resilin and (ii) RSF/poly(N-vinylcaprolactam (PVCL) is reported for the first time using small-angle scattering (SAS) techniques. The structure of RSF in dilute to concentrated solution to fabricated hydrogels were characterized using small angle X-ray scattering (SAXS), small angle neutron scattering (SANS) and ultra-small angle neutron scattering (USANS) techniques. The RSF hydrogel exhibited three distinctive structural characteristics: (i) a Porod region in the length scale of 2 to 3 nm due to hydrophobic domains (containing β-sheets) which exhibits sharp interfaces with the amorphous matrix of the hydrogel and the solvent, (ii) a Guinier region in the length scale of 4 to 20 nm due to hydrophilic domains (containing turns and random coil), and (iii) a Porod-like region in the length scale of few micrometers due to water pores/channels exhibiting fractal-like characteristics. Addition of Rec1-resilin or PVCL to RSF and subsequent crosslinking systematically increased the nanoscale size of hydrophobic and hydrophilic domains, whereas decreased the homogeneity of pore size distribution in the microscale. The presented results have implications on the fundamental understanding of the structure–property relationship of RSF-based hydrogels. © 2018 Elsevier B.V.en_AU
dc.description.sponsorshipThis research has been financially supported by the Australian Research Council (ARC) through Discovery Grant funding (DP160101267 and DP120103537). The SAXS, SANS and USANS experiments were supported by the ANSTO beam time award (P3550).en_AU
dc.identifier.citationWhittaker, J. L., Balu, R., Knott, R., de Campo, L., Mata, J. P., Rehm, C., Hill, A. J., Dutta, N. K., & Choudhury, N. R. (2018). Structural evolution of photocrosslinked silk fibroin and silk fibroin-based hybrid hydrogels: a small angle and ultra-small angle scattering investigation. International Journal of Biological Macromolecules, 114, 998-1007. doi:10.1016/j.ijbiomac.2018.03.044en_AU
dc.identifier.issn0141-8130en_AU
dc.identifier.journaltitleInternational Journal of Biological Macromoleculesen_AU
dc.identifier.pagination998-1007en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15192en_AU
dc.identifier.volume114en_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.relation.urihttps://doi.org/10.1016/j.ijbiomac.2018.03.044en_AU
dc.subjectSmall angle scatteringen_AU
dc.subjectHydrogelsen_AU
dc.subjectProteinsen_AU
dc.subjectNeutron diffractionen_AU
dc.subjectSolventsen_AU
dc.subjectMicrostructureen_AU
dc.titleStructural evolution of photocrosslinked silk fibroin and silk fibroin-based hybrid hydrogels: a small angle and ultra-small angle scattering investigationen_AU
dc.typeJournal Articleen_AU
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