Natural polyelectrolyte films based on layer-by layer deposition of collagen and hyaluronic acid.

The aim of the present work was to assemble extracellular matrix components into polyelectrolyte multilayers using the layer-by-layer deposition method. The films are constructed with type-I collagen and hyaluronic acid. The construction exhibits the general features observed during polyelectrolyte multilayer buildup: alternate positive and negative values of the zeta potential of the film during its construction and regular increase of the film thickness with the number, n, of deposition step. This increase is shown to be linear with n. As expected for a linearly growing film, the confocal microscopy shows that when the film is brought in contact with a collagen solution, collagen does not diffuse into the film but interacts only with its outer layer. However, the films are not constituted of homogeneously distributed polyanion/polycation complexes as it is usually observed, but they are formed of fibers as imaged by AFM. The typical width of these fibers increases with the number of deposition steps. Finally, it is found that chondrosarcoma cells spread well and synthesize extracellular matrix components only on the collagen ending films, whereas no cellular matrix was found for HA ending ones. Such architectures may be further functionalized by inclusion of active drugs, peptides, proteins..., and could be used as tunable biomaterial interfaces.

[1]  E. Balazs,et al.  The chemistry, biology and medical applications of hyaluronan and its derivatives , 1998 .

[2]  M. Balasubramani,et al.  Skin substitutes: a review. , 2001, Burns : journal of the International Society for Burn Injuries.

[3]  L. Richert,et al.  Improvement of stability and cell adhesion properties of polyelectrolyte multilayer films by chemical cross-linking. , 2004, Biomacromolecules.

[4]  G. Prestwich,et al.  Molecular basis for the explanation of the exponential growth of polyelectrolyte multilayers , 2002, Proceedings of the National Academy of Sciences of the United States of America.

[5]  Ali Khademhosseini,et al.  Layer-by-layer deposition of hyaluronic acid and poly-L-lysine for patterned cell co-cultures. , 2004, Biomaterials.

[6]  Alain M. Jonas,et al.  Ultrathin polymer coatings by complexation of polyelectrolytes at interfaces: suitable materials, structure and properties , 2000 .

[7]  F. Caruso,et al.  Growth of multilayer films of fixed and variable charge density polyelectrolytes: Effect of mutual charge and secondary interactions , 2003 .

[8]  H. Möhwald,et al.  Assembly of polyelectrolyte multilayer films by consecutively alternating adsorption of polynucleotides and polycations , 1996 .

[9]  M. Zembala,et al.  Streaming potential measurements related to fibrinogen adsorption onto silica capillaries , 1994 .

[10]  M. Cynthia Goh,et al.  Atomic Force Microscopy Studies of Salt Effects on Polyelectrolyte Multilayer Film Morphology , 2001 .

[11]  Benjamin Thierry,et al.  Bioactive coatings of endovascular stents based on polyelectrolyte multilayers. , 2003, Biomacromolecules.

[12]  N. Shanmugasundaram,et al.  Collagen-chitosan polymeric scaffolds for the in vitro culture of human epidermoid carcinoma cells. , 2001, Biomaterials.

[13]  Y. Takano,et al.  Establishment of a clonal human chondrosarcoma cell line with cartilage phenotypes. , 1989, Cancer research.

[14]  J. Schlenoff,et al.  Protein adsorption modalities on polyelectrolyte multilayers. , 2004, Biomacromolecules.

[15]  Massoud Motamedi,et al.  Collagen Coating Promotes Biocompatibility of Semiconductor Nanoparticles in Stratified LBL Films , 2003 .

[16]  Heinrich Haas,et al.  X-ray analysis of ultrathin polymer films self-assembled onto substrates , 1994 .

[17]  F. Caruso,et al.  Protein multilayer formation on colloids through a stepwise self-assembly technique. , 1999 .

[18]  Katsuhiko Ariga,et al.  Alternate Assembly of Ordered Multilayers of SiO2 and Other Nanoparticles and Polyions , 1997 .

[19]  Jeffrey A. Hubbell,et al.  Thin Polymer Layers Formed by Polyelectrolyte Multilayer Techniques on Biological Surfaces , 1999 .

[20]  F. Berthod,et al.  Nerve regeneration in a collagen-chitosan tissue-engineered skin transplanted on nude mice. , 2003, Biomaterials.

[21]  Yugyung Lee,et al.  Biomedical applications of collagen. , 2001, International journal of pharmaceutics.

[22]  Benjamin Geiger,et al.  Initial stages of cell-matrix adhesion can be mediated and modulated by cell-surface hyaluronan. , 2002, Biophysical journal.

[23]  C. Barrett,et al.  pH-responsive properties of multilayered poly(L-lysine)/hyaluronic acid surfaces. , 2003, Biomacromolecules.

[24]  A Rajaram,et al.  Influence of different crosslinking treatments on the physical properties of collagen membranes. , 2003, Biomaterials.

[25]  Linshu Liu,et al.  An osteoconductive collagen/hyaluronate matrix for bone regeneration. , 1999, Biomaterials.

[26]  Katsuhiko Ariga,et al.  ASSEMBLY OF MULTICOMPONENT PROTEIN FILMS BY MEANS OF ELECTROSTATIC LAYER-BY-LAYER ADSORPTION , 1995 .

[27]  G. J. Fleer,et al.  Formation and stability of multilayers of polyelectrolytes. , 1996 .

[28]  M. Tabrizian,et al.  Nanocoatings onto arteries via layer-by-layer deposition: toward the in vivo repair of damaged blood vessels. , 2003, Journal of the American Chemical Society.

[29]  Johannes Schmitt,et al.  New nanocomposite films for biosensors: layer-by-layer adsorbed films of polyelectrolytes, proteins or DNA , 1993 .

[30]  Yoshiya Tanaka,et al.  Chondrocytes Are Regulated by Cellular Adhesion Through CD44 and Hyaluronic Acid Pathway , 1997, Journal of bone and mineral research : the official journal of the American Society for Bone and Mineral Research.

[31]  M. V. Voinova,et al.  Viscoelastic Acoustic Response of Layered Polymer Films at Fluid-Solid Interfaces: Continuum Mechanics Approach , 1998, cond-mat/9805266.

[32]  F. Caruso,et al.  2. Assembly of Alternating Polyelectrolyte and Protein Multilayer Films for Immunosensing , 1997 .

[33]  P. Schaaf,et al.  Bioactive Coatings Based on a Polyelectrolyte Multilayer Architecture Functionalized by Embedded Proteins , 2003 .

[34]  G. Prestwich,et al.  Cross-linked hyaluronic acid hydrogel films: new biomaterials for drug delivery. , 2000, Journal of controlled release : official journal of the Controlled Release Society.

[35]  Allon I Hochbaum,et al.  Rational design of cytophilic and cytophobic polyelectrolyte multilayer thin films. , 2003, Biomacromolecules.

[36]  Si-Nae Park,et al.  Biological characterization of EDC-crosslinked collagen-hyaluronic acid matrix in dermal tissue restoration. , 2003, Biomaterials.

[37]  L. Lazzeri,et al.  Bioartificial materials based on blends of collagen and poly(acrylic acid) , 1999 .

[38]  P. Schaaf,et al.  In Situ Determination of the Structural Properties of Initially Deposited Polyelectrolyte Multilayers , 2000 .

[39]  P. Schaaf,et al.  Control of Monocyte Morphology on and Response to Model Surfaces for Implants Equipped with Anti‐Inflammatory Agent , 2004 .

[40]  J. A. Chapman,et al.  Collagen fibril formation. , 1996, The Biochemical journal.

[41]  G. Prestwich,et al.  Layer by layer buildup of polysaccharide films: physical chemistry and cellular adhesion aspects. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[42]  P. Schaaf,et al.  Comparison of the Structure of Polyelectrolyte Multilayer Films Exhibiting a Linear and an Exponential Growth Regime: An in Situ Atomic Force Microscopy Study , 2002 .

[43]  Nicholas A. Kotov,et al.  Layer-By-Layer Assembly of Collagen Thin Films: Controlled Thickness and Biocompatibility , 2001 .

[44]  Catherine Picart,et al.  Buildup Mechanism for Poly(l-lysine)/Hyaluronic Acid Films onto a Solid Surface , 2001 .

[45]  Stefaan De Smedt,et al.  HYALURONAN : PREPARATION, STRUCTURE, PROPERTIES, AND APPLICATIONS , 1998 .

[46]  F. Caruso,et al.  Influence of Polyelectrolyte Multilayer Coatings on Förster Resonance Energy Transfer between 6-Carboxyfluorescein and Rhodamine B-Labeled Particles in Aqueous Solution , 1998 .

[47]  Alyssa Panitch,et al.  Polymeric biomaterials for tissue and organ regeneration , 2001 .

[48]  J. Voegel,et al.  Endothelial cells grown on thin polyelectrolyte mutlilayered films: an evaluation of a new versatile surface modification. , 2003, Biomaterials.