Self-Assembled Hydrogel Fiber Bundles from Oppositely Charged Polyelectrolytes Mimic Micro-/Nanoscale Hierarchy of Collagen

last updated: 2017-08-31
ProjectRECOGNIZE :: publications list
TitleSelf-Assembled Hydrogel Fiber Bundles from Oppositely Charged Polyelectrolytes Mimic Micro-/Nanoscale Hierarchy of Collagen
Publication TypePapers in Scientific Journals
Year of Publication2017
AuthorsSant S., Coutinho D. F., Gaharwar A. K., Neves N. M., Reis R. L., Gomes M. E., and Khademhosseini A.

Fiber bundles are present in many tissues throughout the body. In most cases,
collagen subunits spontaneously self-assemble into a fibrilar structure that
provides ductility to bone and constitutes the basis of muscle contraction.
Translating these natural architectural features into a biomimetic scaffold still
remains a great challenge. Here, a simple strategy is proposed to engineer
biomimetic fiber bundles that replicate the self-assembly and hierarchy of
natural collagen fibers. The electrostatic interaction of methacrylated gellan
gum with a countercharged chitosan polymer leads to the complexation of the
polyelectrolytes. When directed through a polydimethylsiloxane channel, the
polyelectrolytes form a hierarchical fibrous hydrogel demonstrating nanoscale
periodic light/dark bands similar to D-periodic bands in native collagen and
align parallel fibrils at microscale. Importantly, collagen-mimicking hydrogel
fibers exhibit robust mechanical properties (MPa scale) at a single fiber bundle
level and enable encapsulation of cells inside the fibers under cell-friendly mild
conditions. Presence of carboxyl- (in gellan gum) or amino- (in chitosan) functionalities
further enables controlled peptide functionalization such as Arginylglycylaspartic
acid (RGD) for biochemical mimicry (cell adhesion sites) of native
collagen. This biomimetic-aligned fibrous hydrogel system can potentially be
used as a scaffold for tissue engineering as well as a drug/gene delivery vehicle.

JournalAdv. Funct. Mater.
Date Published2017-08-16
Keywordsbottom-up self-assembly, chitosan and gellan gum, collagen mimicking, hierarchical hydrogel fibers, Polyelectrolyte Complexes
Peer reviewedyes

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