Controlled Degradability of Polysaccharide Multilayer Films In Vitro and In Vivo

This article demonstrates the possibility of tuning the degradability of polysaccharide multilayer films in vitro and in vivo. Chitosan and hyaluronan multilayer films (CHI/HA) were either native or crosslinked using a water soluble carbodiimide, 1‐ethyl‐3‐(3‐dimethylamino‐propyl)carbodiimide (EDC) at various concentrations in combination with N‐hydroxysulfosuccinimide. The in‐vitro degradation of the films in contact with lysozyme and hyaluronidase was followed by quartz crystal microbalance measurements, fluorimetry, and confocal laser scanning microscopy after labeling of the chitosan with fluorescein isothiocyanate (CHIFITC). The native films were subjected to degradation by these enzymes, and the crosslinked films were more resistant to enzymatic degradation. Films made of chitosan of medium molecular weight were more resistant than films made of chitosan‐oligosaccharides. The films were also brought in contact with plasma, which induced a change in film structure for the native film but did not have any effect on the crosslinked film. The in‐vitro study shows that macrophages can degrade all types of films and internalize the chitosan. The in‐vivo degradation of the films implanted in mouse peritoneal cavity for a week again showed an almost complete degradation of the native films, whereas the crosslinked films were only partially degraded. Taken together, these results suggest that polysaccharide multilayer films are of potential interest for in‐vivo applications as biodegradable coatings, and that degradation can be tuned by using chitosan of different molecular weights and by controlling film crosslinking.

[1]  D. Ponzin,et al.  Characterization of macrophages elicited by intraperitoneal injection of hyaluronate , 1986, Agents and Actions.

[2]  Y. Arntz,et al.  Primary Cell Adhesion on RGD‐Functionalized and Covalently Crosslinked Thin Polyelectrolyte Multilayer Films , 2005 .

[3]  J. Voegel,et al.  Pyridylamino‐β‐cyclodextrin as a Molecular Chaperone for Lipopolysaccharide Embedded in a Multilayered Polyelectrolyte Architecture , 2004 .

[4]  D. Discher,et al.  Elasticity of native and cross-linked polyelectrolyte multilayer films. , 2004, Biomacromolecules.

[5]  K. M. Faucher,et al.  A membrane-mimetic barrier for islet encapsulation. , 2004, Transplantation proceedings.

[6]  Luhang Zhao,et al.  Receptor-mediated stimulatory effect of oligochitosan in macrophages. , 2004, Biochemical and biophysical research communications.

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

[8]  P. Schaaf,et al.  Build‐up of Polypeptide Multilayer Coatings with Anti‐Inflammatory Properties Based on the Embedding of Piroxicam–Cyclodextrin Complexes , 2004 .

[9]  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.

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

[11]  G. Sukhorukov,et al.  Loading the multilayer dextran sulfate/protamine microsized capsules with peroxidase. , 2003, Biomacromolecules.

[12]  W. J. Wang,et al.  Crosslinked collagen/chitosan matrix for artificial livers. , 2003, Biomaterials.

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

[14]  J. Mao,et al.  Structure and properties of bilayer chitosan-gelatin scaffolds. , 2003, Biomaterials.

[15]  Masanori Fujita,et al.  Controlled release of fibroblast growth factors and heparin from photocrosslinked chitosan hydrogels and subsequent effect on in vivo vascularization. , 2003, Journal of biomedical materials research. Part A.

[16]  H. Möhwald,et al.  Layer-by-layer engineering of biocompatible, decomposable core-shell structures. , 2003, Biomacromolecules.

[17]  M. Rinaudo,et al.  Hydration of polysaccharide hyaluronan observed by IR spectrometry. I. Preliminary experiments and band assignments. , 2003, Biopolymers.

[18]  M. C. Ferreira,et al.  An optimised method to determine the degree of acetylation of chitin and chitosan by FTIR spectroscopy. , 2002, International journal of biological macromolecules.

[19]  S. Elder,et al.  Potential use of chitosan as a cell scaffold material for cartilage tissue engineering. , 2002, Tissue engineering.

[20]  D. M. Lynn,et al.  Construction of hydrolytically-degradable thin films via layer-by-layer deposition of degradable polyelectrolytes. , 2002, Journal of the American Chemical Society.

[21]  M. Akashi,et al.  Enzymatic Hydrolysis of a Layer-by-Layer Assembly Prepared from Chitosan and Dextran Sulfate , 2002 .

[22]  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.

[23]  G. Prestwich,et al.  Glycosaminoglycan hydrogel films as bio-interactive dressings for wound healing. , 2002, Biomaterials.

[24]  J. Desbrières,et al.  Influence of the nature of the metal ions on the complexation with chitosan.: Application to the treatment of liquid waste , 2002 .

[25]  M. Akashi,et al.  Alternating bioactivity of polymeric layer-by-layer assemblies: anticoagulation vs procoagulation of human blood. , 2002, Biomacromolecules.

[26]  Nicholas A. Kotov,et al.  Biomaterials by Design: Layer‐By‐Layer Assembled Ion‐Selective and Biocompatible Films of TiO2 Nanoshells for Neurochemical Monitoring , 2002 .

[27]  J. Desbrières,et al.  Viscosity of semiflexible chitosan solutions: influence of concentration, temperature, and role of intermolecular interactions. , 2002, Biomacromolecules.

[28]  Steve Granick,et al.  Layered, erasable polymer multilayers formed by hydrogen-bonded sequential self-assembly , 2002 .

[29]  T. Fujinaga,et al.  Topical formulations and wound healing applications of chitosan. , 2001, Advanced drug delivery reviews.

[30]  P. Schaaf,et al.  Stabilizing Effects of Various Polyelectrolyte Multilayer Films on the Structure of Adsorbed/Embedded Fibrinogen Molecules: An ATR-FTIR Study † , 2001 .

[31]  H. Saimoto,et al.  Biological activities of carbohydrate-branched chitosan derivatives. , 2001, Biomacromolecules.

[32]  F. Caruso,et al.  Decomposable hollow biopolymer capsules. , 2001 .

[33]  J. Chluba,et al.  Peptide hormone covalently bound to polyelectrolytes and embedded into multilayer architectures conserving full biological activity. , 2001, Biomacromolecules.

[34]  J. Schlenoff,et al.  Polyelectrolyte Multilayers Containing a Weak Polyacid: Construction and Deconstruction , 2001 .

[35]  J. Suh,et al.  Application of chitosan-based polysaccharide biomaterials in cartilage tissue engineering: a review. , 2000, Biomaterials.

[36]  M. N. R. Kumar.  A review of chitin and chitosan applications , 2000 .

[37]  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.

[38]  L. Block,et al.  Chitosan as an enabling excipient for drug delivery systems. I. Molecular modifications. , 2000, International journal of biological macromolecules.

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

[40]  Paula T. Hammond,et al.  Recent explorations in electrostatic multilayer thin film assembly , 1999 .

[41]  G. Prestwich,et al.  Synthesis and selective cytotoxicity of a hyaluronic acid-antitumor bioconjugate. , 1999, Bioconjugate chemistry.

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

[43]  Brzezinski,et al.  Measurements Using the Quartz Crystal Microbalance Technique of Ferritin Monolayers on Methyl-Thiolated Gold: Dependence of Energy Dissipation and Saturation Coverage on Salt Concentration. , 1998, Journal of colloid and interface science.

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

[45]  E. Menzel,et al.  Hyaluronidase and its substrate hyaluronan: biochemistry, biological activities and therapeutic uses. , 1998, Cancer letters.

[46]  G. Prestwich,et al.  Controlled chemical modification of hyaluronic acid: synthesis, applications, and biodegradation of hydrazide derivatives. , 1998, Journal of controlled release : official journal of the Controlled Release Society.

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

[48]  Y. Ikada,et al.  Crosslinking of hyaluronic acid with water-soluble carbodiimide. , 1997, Journal of biomedical materials research.

[49]  Q. Myrvik,et al.  Chitin particle-induced cell-mediated immunity is inhibited by soluble mannan: mannose receptor-mediated phagocytosis initiates IL-12 production. , 1997, Journal of immunology.

[50]  Gero Decher,et al.  Fuzzy Nanoassemblies: Toward Layered Polymeric Multicomposites , 1997 .

[51]  Y Ikada,et al.  In vitro and in vivo degradation of films of chitin and its deacetylated derivatives. , 1997, Biomaterials.

[52]  R. Muzzarelli,et al.  Human enzymatic activities related to the therapeutic administration of chitin derivatives , 1997, Cellular and Molecular Life Sciences CMLS.

[53]  Bengt Herbert Kasemo,et al.  A simple setup to simultaneously measure the resonant frequency and the absolute dissipation factor of a quartz crystal microbalance , 1996 .

[54]  J. Desbrières,et al.  Hydrophobic derivatives of chitosan: characterization and rheological behaviour. , 1996, International journal of biological macromolecules.

[55]  Alain Domard,et al.  Chitosan-chondroitin sulfate and chitosan-hyaluronate polyelectrolyte complexes. Physico-chemical aspects , 1996 .

[56]  O. Smidsrod,et al.  Degradation of partially N-acetylated chitosans with hen egg white and human lysozyme , 1996 .

[57]  G. Hermanson.  3 – Zero-Length Cross-linkers , 1996 .

[58]  E. Veerman,et al.  Biochemical composition of human saliva in relation to other mucosal fluids. , 1995, Critical reviews in oral biology and medicine : an official publication of the American Association of Oral Biologists.

[59]  M. Otterlei,et al.  Characterization of binding and TNF-alpha-inducing ability of chitosans on monocytes: the involvement of CD14. , 1994, Vaccine.

[60]  M. Rinaudo,et al.  Characterization of chitosan. Influence of ionic strength and degree of acetylation on chain expansion. , 1993, International journal of biological macromolecules.

[61]  M. Rinaudo,et al.  Influence of the ionic strength on the dimensions of sodium hyaluronate , 1992 .

[62]  Johannes Schmitt,et al.  Buildup of ultrathin multilayer films by a self-assembly process: III. Consecutively alternating adsorption of anionic and cationic polyelectrolytes on charged surfaces , 1992 .

[63]  M. Yamada,et al.  Purification of hyaluronidase from human placenta. , 1977, Journal of biochemistry.