Skip to main content
SpringerLink
Log in

Directed Mineralization on Polyelectrolyte Multilayer Films

  • Published:
MRS Online Proceedings Library Aims and scope

Abstract

Silica formation aided by polypeptides is being actively investigated for a wide range of applications including biomaterials synthesis, ceramics and controlled release systems. We envision that biocatalyzed mineralization could have application as a dental material wherein situ formation of mineral layers could provide needed wear-resistance or sealing capability. The approach would be more clinically relevant, if a polymer host could be used to carry and specifically position the biocatalyst on a surface and additionally maintain the catalyst activity.

Accordingly, we studied the influence of simple catalytic polypeptides on silica formation from prehydrolyzed alkoxide precursor solutions onto a surface. The polypeptides were localized on to the surface as multilayered thin films using the layer-by-layer (LbL) assembly of polyelectrolytes. Polylysine (PLL) or another biocatalytic polycation, poly(ethyleneimine) (PEI), was adsorbed layer-by-layer up to 10 bilayers on silicon wafers in combination with a negatively charged polyelectrolyte polymer host, poly(sodium-4-styrene sulfonate) (PSS) to prepare PEI-(PLL/PSS)10, PEI-(PEI/PSS)10 and PEI-(PEI/PSS/PLL/PSS)10 multilayer films. Pre-hydrolyzed alkoxysilane solutions were placed dropwise on the catalytic films for silicification. Additionally, the effects of precursor concentration, solvent and drying were evaluated. The morphology, roughness and contact mechanical stiffness of the formed silica were investigated using optical microscopy (OM), scanning electron microscopy (SEM) and atomic force microscopy (AFM).

The resulting silica morphology was plate-like or spherical, and porous with average particle size depending on the catalyst and its positions on the surface. Without a catalyst the silica formed over longer times with a fine, gel-like appearance. The morphology of silica produced on the substrate was different from that of particles catalyzed in solution with the same polypeptide catalyst. Additionally, it was found that the homogeneity of PEI-(PLL/PSS)10 films increased with drying temperature, silica precursor concentration and the presence of ethanol. The contact mechanical stiffness of the silica particles (40 N/m) catalyzed from PEI-(PLL/PSS)10 films was lower than the non-silicified areas (48 N/m) suggesting that regions of the silica were amorphous and hydrated. These results show that a polypeptide applied to a surface as a multiple layer with an oppositely charged polymer host (PSS) maintains its activity for silicification. The generally coherent nature of the mineral coating suggests its potential for enhancing critical restorative dental interfaces; however properties like porosity, hydration and their effect on hardness and permeability will need further study.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. N. Kroger, R. Deutzmann, M. Sumper, Science 286, 1129 (1999).

    Article  CAS  Google Scholar 

  2. P. J. Lopez, C. Gautier, J. Livage, T. Coradin, Current Nanoscience 1, 73 (2005).

    Article  CAS  Google Scholar 

  3. S. Mann, G. Ozin, Nature 382, 313 (1996).

    Article  CAS  Google Scholar 

  4. S. V. Patwardhan, S. Clarson, Silicon Chemistry 1, 207 (2002).

    Article  CAS  Google Scholar 

  5. T. Coradin, J. Livage, Colloids and Surfaces B: Biointerfaces 21, 329 (2001).

    Article  CAS  Google Scholar 

  6. S. V. Patwardhan, N. Mukherjee, S. Clarson, J. Inorganic and Organometallic Polymers 11, 193 (2001).

    Article  CAS  Google Scholar 

  7. S. V. Patwardhan, N. Mukherjee, S. J. Clarson, Silicon Chemistry 1, 47 (2002).

    Article  CAS  Google Scholar 

  8. F. Rodriguez, D. D. Glawe, R. R. Naik, K. P. Hallinan, M. O. Stone, Biomacromolecules 5, 261 (2004).

    Article  CAS  Google Scholar 

  9. M. Tomczak et al., J. Am. Chem. Soc. 126, 12 (2005).

    Google Scholar 

  10. T. Coradin, A. Marchalo, N. Abdoul-Aribi, J. Livage, Colloids and Surfaces B: Biointerfaces 44, 191 (2005).

    Article  CAS  Google Scholar 

  11. R. T. Butler, N. J. Ferrell, D. J. Hansford, Applied Surface Science 1, 1 (2005).

    Google Scholar 

  12. R. R. Naik et al., Progress in Organic Coatings 47, 249 (2003).

    Article  CAS  Google Scholar 

  13. M. Advincula, R. Advincula, J. Lemons, Polymer Preprints (ACS) 45, 496 (2004).

    CAS  Google Scholar 

  14. C. Lefaux, J. Zimberlin, A. Dobrynin, P. T. Mather, J. Polymer Sci. Part B: Polym. Phys. 42, 3654 (2004).

    Article  CAS  Google Scholar 

  15. X. Shi, M. Shen, H. Mohwald, Prog. Polym. Sci. 29, 987 (2004).

    Article  CAS  Google Scholar 

  16. Y. Lvov, K. Ariga, I. Ichinose, T. Kunitake, J. Am. Chem. Soc. 117, 6117 (1995).

    Article  CAS  Google Scholar 

  17. N. Nakabayashi, N. Honda, J. Japan. Soc. Den. Mat. 6, 873 (1987).

    Google Scholar 

  18. Y. Zhang, K. Agee, D. H. Pashley, E. L. Pashley, J. Clin. Periodontol. 25, 884 (1998).

    Article  CAS  Google Scholar 

  19. J. Cha et al., Proc. Natl. Acad. Sci. 96, 361 (1999).

    Article  CAS  Google Scholar 

  20. C. J. Brinker, G. W. Scherer, Sol-gel Science: The Physics and Chemistry of Sol-Gel Processing (Academic Press, Inc., New York, 1990).

Download references

Author information

Authors and Affiliations

  1. Oral Rehabilitation, University of Connecticut Health Center, MC-1615, 263 Farmington Ave, Farmington, CT, 06030, USA

    Maria C. Advincula & A. Jon Goldberg

  2. Macromolecular Science and Engineering, Case Western Reserve University, 312 Kent Hale Smith Building, 2100 Adelbert Road, Cleveland, OH, 44106, USA

    Pritesh A. Patel & Patrick T. Mather

  3. Institute of Materials Science, University of Connecticut, 97 North Eagleville Road, Storrs, CT, 06269, USA

    Daniel Underhill & Bryan D. Huey

Authors
  1. Maria C. Advincula
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Pritesh A. Patel
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Patrick T. Mather
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Daniel Underhill
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Bryan D. Huey
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. A. Jon Goldberg
    View author publications

    You can also search for this author in PubMed Google Scholar

Rights and permissions

Reprints and permissions

About this article

Cite this article

Advincula, M.C., Patel, P.A., Mather, P.T. et al. Directed Mineralization on Polyelectrolyte Multilayer Films. MRS Online Proceedings Library 975, 603 (2006). https://doi.org/10.1557/PROC-975-0975-DD06-03

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1557/PROC-975-0975-DD06-03

Search

Navigation