Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 27, Issue 36, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201606273
Keywords
bottom-up self-assembly; chitosan and gellan gum; collagen mimicking; hierarchical hydrogel fibers; polyelectrolyte complexes
Categories
Funding
- US Army Engineer Research and Development Center
- Institute for Soldier Nanotechnology
- NIH [HL092836, EB007249]
- National Science Foundation CAREER award
- POCTI and/or FEDER programs
- European Union under the project NoE EXPERTISSUES [NMP3-CT-2004-500283]
- Foundation for Science and Technology (FCT), Portugal
- MIT-Portugal Program [SFRH/BD/37156/2007]
- Le Fonds Quebecois de la Recherche sur la Nature et les Technologies (FQRNT), Quebec, Canada
- System-based Consortium for Organ Design and Engineering (SysCODE) [NIH NRSA T32]
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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.
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