Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

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.

This is a preview of subscription content, access via your institution

Access options

Rent or buy this article

Prices vary by article type

from$1.95

to$39.95

Prices may be subject to local taxes which are calculated during checkout

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.

Similar content being viewed by others

References

  1. Pilnik, W. & Rombouts, F. M. Polysaccharides and food processing. Carbohydr. Res. 142, 93–105 (1985)

    Article  CAS  Google Scholar 

  2. Peppas, N. A., Hilt, J. Z., Khademhosseini, A. & Langer, R. Hydrogels in biology and medicine: From molecular principles to bionanotechnology. Adv. Mater. 18, 1345–1360 (2006)

    Article  CAS  Google Scholar 

  3. Drury, J. L. & Mooney, D. J. Hydrogels for tissue engineering: scaffold design variables and applications. Biomaterials 24, 4337–4351 (2003)

    Article  CAS  Google Scholar 

  4. Montembault, A., Viton, C. & Domard, A. Physico-chemical studies of the gelation of chitosan in a hydroalcoholic medium. Biomaterials 26, 933–943 (2005)

    Article  CAS  Google Scholar 

  5. Varum, K. M., Myhr, M. M., Hjerde, R. J. & Smidsrod, O. In vitro degradation rates of partially N-acetylated chitosans in human serum. Carbohydr. Res. 299, 99–101 (1997)

    Article  CAS  Google Scholar 

  6. Domard, A. & Domard, M. in Polymeric Biomaterials (ed. Dimitriu, S.) 187–212 (2002)

    Google Scholar 

  7. Hirano, S. & Noishiki, Y. The blood biocompatibility of chitosan and N-acetylchitosans. J. Biomed. Mater. Res. 19, 413–417 (1985)

    Article  CAS  Google Scholar 

  8. Lamarque, G., Lucas, J.-M., Viton, C. & Domard, A. Physicochemical behavior of homogeneous series of acetylated chitosans in aqueous solution: role of various structural parameters. Biomacromolecules 6, 131–142 (2005)

    Article  CAS  Google Scholar 

  9. Schatz, C., Viton, C., Delair, T., Pichot, C. & Domard, A. Typical physicochemical behaviors of chitosans in aqueous solution. Biomacromolecules 4, 641–648 (2003)

    Article  CAS  Google Scholar 

  10. Sorlier, P., Denuziere, A., Viton, C. & Domard, A. Relation between the degree of acetylation and the electrostatic properties of chitin and chitosan. Biomacromolecules 2, 765–772 (2001)

    Article  CAS  Google Scholar 

  11. Malette, W. G., Quigley, H. J., Gaines, R. D., Johnson, N. D. & Rainer, W. G. Chitosan, a new haemostatic. Ann. Thorac. Surg. 36, 55–61 (1983)

    Article  CAS  Google Scholar 

  12. Strand, S. P., Vandik, M. S., Varum, K. J. & Ostgaard, K. Screening of chitosans and conditions for bacterial flocculation. Biomacromolecules 2, 126–133 (2001)

    Article  CAS  Google Scholar 

  13. Montembault, A. et al. A material decoy of biological media based on chitosan physical hydrogels: applications to cartilage tissue engineering. Biochimie 88, 551–564 (2006)

    Article  CAS  Google Scholar 

  14. Boucard, N. et al. The use of physical hydrogels of chitosan for skin regeneration following third-degree burns. Biomaterials 28, 3478–3488 (2007)

    Article  CAS  Google Scholar 

  15. Boucard, N., Viton, C. & Domard, A. New aspect of the formation of physical hydrogels of chitosan in a hydroalcoholic medium. Biomacromolecules 6, 3227–3237 (2005)

    Article  CAS  Google Scholar 

  16. Vasquez, B., Gurruchaga, M., Goni, I. & San Roman, J. pH-sensitive hydrogel based on non-ionic acrylic copolymers. Biomaterials 18, 521–526 (1997)

    Article  Google Scholar 

  17. Ilmain, F., Tanaka, T. & Kokufuta, E. Volume transition in a gel driven by hydrogen bonding. Nature 349, 400–401 (1991)

    Article  ADS  CAS  Google Scholar 

  18. Siegel, R. A. & Firestone, B. A. pH dependent equilibrium swelling properties of hydrophobic polyelectrolytes copolymers gels. Macromolecules 21, 3254–3259 (1988)

    Article  ADS  CAS  Google Scholar 

  19. Ostroha, J., Pong, M., Lowman, A. & Dan, N. Controlling the collapse swelling transition in charged hydrogels. Biomaterials 25, 4345–4353 (2004)

    Article  CAS  Google Scholar 

  20. Porath, J., Sundberg, L., Fornstedt, N. & Olsson, I. Salting-out in amphiphilic gels as new approach to hydrophobic adsorption. Nature 245, 465–466 (1973)

    Article  ADS  CAS  Google Scholar 

  21. Von Hippel, P. H. & Schleich, T. Ions effect on the solution of biological macromolecules. Acc. Chem. Res. 2, 257–265 (1969)

    Article  CAS  Google Scholar 

  22. Pu, Q., Ng, S., Mok, V. & Chen, S. B. Ion bridging effects on the electroviscosity of flexible polyelectrolytes. J. Phys. Chem. B 108, 14124–14129 (2004)

    Article  CAS  Google Scholar 

Download references

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.

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Laurent David or Alain Domard.

Supplementary information

Supplementary Information

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

Rights and permissions

Reprints and permissions

About this article

Cite this article

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

Download citation

  • Received:

  • Accepted:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nature06619

This article is cited by

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing