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Silk fibroin dissolution in Tetrabutylammonium hydroxide aqueous solution

2019-11Journal article Restricted access
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dc.contributor.authorMedronho, Bruno
dc.contributor.authorFilipe, Alexandra
dc.contributor.authorNapso, Sofia
dc.contributor.authorKhalfin, Rafail. L.
dc.contributor.authorPereira, Rui F. P.
dc.contributor.authorBermudez, Vermica de Zea
dc.contributor.authorRomano, Anabela
dc.contributor.authorCohen, Yachin
dc.date.accessioned2020-07-24T10:51:03Z
dc.date.available2020-07-24T10:51:03Z
dc.date.issued2019-11
dc.description.abstractBombyx mori L. silk fibroin (SF) is widely used in different areas due to its ability to form durable and resilient materials with notable mechanical properties. However, in some of these applications the dissolution of SF is required, and this is not often straightforward due to its inability to be dissolved in the majority of common solvents. This work reports a novel approach to dissolve SF using 40 wt % aqueous tetrabutylammonium hydroxide, TBAOH(aq), at mild temperature. A thorough rheological study combined with small-angle X-ray scattering is presented to correlate the SF state in solution with changes in the rheological parameters. The scattering data suggest that the SF conformation in TBAOH(aq) is close to a random coil, possibly having some compact domains linked with flexible random chains. The radius of gyration (R-g) and the molecular weight (M-w) were estimated to be ca. 17.5 nm and 450 kDa, respectively, which are in good agreement with previous works. Nevertheless, a lower M-w value was deduced from rheometry (i.e., 321 kDa) demonstrating a low degree of depolymerization during dissolution in comparison to other harsh processes. The transition from a dilute to a semidilute regime coincides with the estimated critical concentration and is marked by the presence of a shear-thinning behavior in the flow curves, violation of the empirical Cox-Merz rule, and an upward increase in the activation energy. This work paves the way toward the development of advanced high-tech SF-based materials.
dc.description.sponsorshipPortuguese Foundation for Science and Technology, FCTPortuguese Foundation for Science and Technology [PTDC/AGR-TEC/4814/2014, PTDC/ASP-SIL/30619/2017, UID/QUI/00686/2019, POCI-01-0145-FEDER-016884, PTDC/CTM-NAN/0956/2014]
dc.description.sponsorshipUniRCell project [SAICTPAC/0032/2015, POCI-01-0145-FEDER-016422, IF/01005/2014, 57/2017]
dc.description.versioninfo:eu-repo/semantics/publishedVersion
dc.identifier.doi10.1021/acs.biomac.9b00946
dc.identifier.issn1525-7797
dc.identifier.urihttp://hdl.handle.net/10400.1/14190
dc.language.isoeng
dc.peerreviewedyes
dc.publisherAmerican Chemical Society
dc.subjectBombyx-mori
dc.subjectMolecular-weight
dc.subjectCellulose dissolution
dc.subjectViscosity
dc.subjectStrength
dc.subjectRegeneration
dc.subjectDependence
dc.subjectDiffusion
dc.subjectToughness
dc.subjectSolvents
dc.titleSilk fibroin dissolution in Tetrabutylammonium hydroxide aqueous solution
dc.typejournal article
dspace.entity.typePublication
oaire.citation.endPage4116
oaire.citation.issue11
oaire.citation.startPage4107
oaire.citation.titleBiomacromolecules
oaire.citation.volume20
person.familyNameMedronho
person.familyNameRomano
person.givenNameBruno
person.givenNameAnabela
person.identifier.ciencia-id6918-9AB3-8D22
person.identifier.ciencia-id8A18-7E9A-3B0E
person.identifier.orcid0000-0003-0972-1739
person.identifier.orcid0000-0002-7204-7428
person.identifier.ridP-5927-2014
person.identifier.scopus-author-id9940656700
person.identifier.scopus-author-id56249997600
rcaap.rightsrestrictedAccess
rcaap.typearticle
relation.isAuthorOfPublication4c03571a-93da-4504-8acf-c74326449852
relation.isAuthorOfPublicatione3343b60-17d3-4f5e-a2bf-06f26da69206
relation.isAuthorOfPublication.latestForDiscovery4c03571a-93da-4504-8acf-c74326449852

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