Particle Diffusivity and Free-Energy Profiles in Hydrogels from Time-Resolved Penetration Data

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dc.contributor.authorWolde-Kidan, Amanuel
dc.contributor.authorHerrmann, Anna
dc.contributor.authorPrause, Albert
dc.contributor.authorGradzielski, Michael
dc.contributor.authorHaag, Rainer
dc.contributor.authorBlock, Stephan
dc.contributor.authorNetz, Roland R.
dc.date.accessioned2021-11-20T06:12:23Z
dc.date.available2021-11-20T06:12:23Z
dc.date.issued2021-01-07
dc.description.abstractA combined experimental and theoretical method to simultaneously determine diffusivity and free-energy profiles of particles that penetrate into inhomogeneous hydrogel systems is presented. As the only input, arbitrarily normalized concentration profiles from fluorescence intensity data of labeled tracer particles for different penetration times are needed. The method is applied to dextran molecules of varying size that penetrate into hydrogels of polyethylene-glycol chains with different lengths that are covalently cross-linked by hyperbranched polyglycerol hubs. Extracted dextran bulk diffusivities agree well with fluorescence correlation spectroscopy data obtained separately. Empirical scaling laws for dextran diffusivities and free energies inside the hydrogel are identified as a function of the dextran mass. An elastic free-volume model that includes dextran as well as polyethylene-glycol linker flexibility quantitively describes the repulsive dextran-hydrogel interaction free energy, which is of steric origin, and furthermore suggests that the hydrogel mesh-size distribution is rather broad and particle penetration is dominated by large hydrogel pores. Particle penetration into hydrogels for steric particle-hydrogel interactions is thus suggested to be governed by an elastic size-filtering mechanism that involves the tail of the hydrogel pore-size distribution.en
dc.description.sponsorshipDFG, 174776315, FOR 1557: Simulation and Evaluation of Acoustical Environments (SEACEN)en
dc.identifier.eissn1542-0086
dc.identifier.issn0006-3495
dc.identifier.pmid33421414en
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/13917
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-12691
dc.language.isoen
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/en
dc.subject.ddc570 Biowissenschaften; Biologieen
dc.subject.othermucusen
dc.subject.otherhydrogelen
dc.subject.otherparticleen
dc.subject.otherdiffusivityen
dc.subject.otherfree-energy profileen
dc.titleParticle Diffusivity and Free-Energy Profiles in Hydrogels from Time-Resolved Penetration Dataen
dc.typeArticleen
dc.type.versionpublishedVersionen
dcterms.bibliographicCitation.doi10.1016/j.bpj.2020.12.020
dcterms.bibliographicCitation.issue3
dcterms.bibliographicCitation.journaltitleBiophysical Journalen
dcterms.bibliographicCitation.originalpublishernameElsevieren
dcterms.bibliographicCitation.originalpublisherplaceAmsterdam [u.a.]en
dcterms.bibliographicCitation.pageend475
dcterms.bibliographicCitation.pagestart463
dcterms.bibliographicCitation.volume120
tub.accessrights.dnbfreeen
tub.affiliationFak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Physikalische Chemie / Molekulare Materialwissenschaftende
tub.affiliation.facultyFak. 2 Mathematik und Naturwissenschaftende
tub.affiliation.groupFG Physikalische Chemie / Molekulare Materialwissenschaftende
tub.affiliation.instituteInst. Chemiede
tub.publisher.universityorinstitutionTechnische Universität Berlinen

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