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Multi-membrane hydrogels

Abstract

Polysaccharide-based hydrogels are useful for numerous applications, from food1 and cosmetic processing to drug delivery and tissue engineering2,3. The formation of hydrogels from polyelectrolyte solutions is complex, involving a variety of molecular interactions. The physical gelation of polysaccharides can be achieved by balancing solvophobic and solvophilic interactions4. Polymer chain reorganization can be obtained by solvent exchange, one of the processing routes forming a simple hydrogel assembly. Nevertheless, many studies on hydrogel formation are empirical with a limited understanding of the mechanisms involved, delaying the processing of more complex structures. Here we use a multi-step interrupted gelation process in controlled physico-chemical conditions to generate complex hydrogels with multi-membrane ‘onion-like’ architectures. Our approach greatly simplifies the processing of gels with complex shapes and a multi-membrane organization. In contrast with existing assemblies described in the literature, our method allows the formation of free ‘inter-membrane’ spaces well suited for cell or drug introduction. These architectures, potentially useful in biomedical applications, open interesting perspectives by taking advantage of tailor-made three-dimensional multi-membrane tubular or spherical structures.

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Figure 1: Multi-membrane hydrogels.
Figure 2: Parameters influencing the polymer mass fraction of physical gels based on chitosan.
Figure 3: Schematic representation of neutralization of a polyelectrolyte alcohol gel and derived methodology for building a multi-membrane structure.
Figure 4: Versatility of the multi-membrane architecture process.

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Acknowledgements

We thank M.-T. Corvol and K. Tahiri (Univ. Paris Descartes) for the chondrocyte cell culture study, and L. Bordenave and R. Bareille (Univ. Victor Segalen, Bordeaux) for additional endothelial/osteoprogenitor cell co-culture experiments. We also thank C. Viton, J.-M. Lucas and A. Crepet for technical assistance, and D. Gillet from Mahtani Chitosan for providing chitosan samples.

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Correspondence to Laurent David or Alain Domard.

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The file contains Supplementary Table S1 and Supplementary Figures S1-S4 with Legends. (PDF 532 kb)

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Ladet, S., David, L. & Domard, A. Multi-membrane hydrogels. Nature 452, 76–79 (2008). https://doi.org/10.1038/nature06619

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