Abstract:
:Hydrogels constructed from folded protein domains are of increasing interest as resilient and responsive biomaterials, but their optimization for applications requires time-consuming and costly molecular design. Here, we explore a complementary approach to control their properties by examining the influence of crosslinking rate on the structure and viscoelastic response of a model hydrogel constructed from photochemically crosslinked bovine serum albumin (BSA). Gelation is observed to follow a heterogeneous nucleation pathway in which BSA monomers crosslink into compact nuclei that grow into fractal percolated networks. Both the viscoelastic response probed by shear rheology and the nanostructure probed by small-angle X-ray scattering (SAXS) are shown to depend on the photochemical crosslinking reaction rate, with increased reaction rates corresponding to higher viscoelastic moduli, lower fractal dimension, and higher fractal cluster size. Reaction rate-dependent changes are shown to be consistent with a transition between diffusion- and rate-limited assembly, and the corresponding changes to viscoelastic response are proposed to arise from the presence of nonfractal depletion regions, as confirmed by SAXS. This controllable nanostructure and viscoelasticity constitute a potential route for the precise control of hydrogel properties, without the need for molecular modification.
journal_name
Biomacromoleculesjournal_title
Biomacromoleculesauthors
Aufderhorst-Roberts A,Hughes MDG,Hare A,Head DA,Kapur N,Brockwell DJ,Dougan Ldoi
10.1021/acs.biomac.0c01044subject
Has Abstractpub_date
2020-10-12 00:00:00pages
4253-4260issue
10eissn
1525-7797issn
1526-4602journal_volume
21pub_type
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journal_title:Biomacromolecules
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journal_title:Biomacromolecules
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journal_title:Biomacromolecules
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pub_type: 杂志文章
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更新日期:2013-04-08 00:00:00
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