Nanomechanical properties of hybrid coatings for bone tissue engineering.

Bone tissue engineering has emerged as a promising alternative approach in the treatment of bone injuries and defects arising from malformation, osteoporosis, and tumours. In this approach, a temporary scaffold possessing mechanical properties resembling those of natural bone is needed to serve as a substrate enhancing cell adhesion and growth, and a physical support to guide the formation of the new bone. In this regard, the scaffold should be biocompatible, biodegradable, malleable and mechanically strong. Herein, we investigate the mechanical properties of three coatings of different chemical compositions onto silanized glass substrates; a hybrid material consisting of methacryloxypropyl trimethoxysilane and zirconium propoxide, a type of a hybrid organic-inorganic material of the above containing also 50 mol% 2-(dimethylamino)ethyl methacrylate (DMAEMA) moieties and a pure organic material, based on PDMAEMA. This study investigates the variations in the measured hardness and reduced modulus values, wear resistance and plastic behaviour before and after samples' submersion in cell culture medium. Through this analysis we aim to explain how hybrid materials behave under applied stresses (pile-up formations), how water uptake changes this behaviour, and estimate how these materials will react while interaction with cells in tissue engineering applications. Finally, we report on the pre-osteoblastic cell adhesion and proliferation on three-dimensional structures of the hybrid materials within the first hour and up to 7 days in culture. It was evident that hybrid structure, consisting of 50 mol% organic-inorganic material, reveals good mechanical behaviour, wear resistance and cell adhesion and proliferation, suggesting a possible candidate in bone tissue engineering.

[1]  C. Bardin,et al.  Subcutaneous hydrogel reservoir system for controlled drug delivery , 1996 .

[2]  S. Armes,et al.  Effect of Partial Quaternization on the Aqueous Solution Properties of Tertiary Amine-Based Polymeric Surfactants: Unexpected Separation of Surface Activity and Cloud Point Behavior , 2001 .

[3]  H. Gleiter,et al.  Nanostructured materials: basic concepts and microstructure☆ , 2000 .

[4]  R. Corriu,et al.  RECENT DEVELOPMENTS OF MOLECULAR CHEMISTRY FOR SOL-GEL PROCESSES , 1996 .

[5]  M. Anglada,et al.  Contact Deformation Regimes Around Sharp Indentations and the Concept of the Characteristic Strain , 2002 .

[6]  M. Munawar Chaudhri,et al.  Accurate determination of the mechanical properties of thin aluminum films deposited on sapphire flats using nanoindentations , 1999 .

[7]  J. E. Chisham,et al.  Sol-gel integrated optical coupler by ultraviolet light imprinting , 1995 .

[8]  C. Brinker Sol-gel science , 1990 .

[9]  C. Charitidis,et al.  Nanoindentation and nanoscratching studies of amorphous carbon films , 1999 .

[10]  G. Pharr,et al.  On the Measurement of Creep by Nanoindentation with Continuous Stiffness Techniques , 2004 .

[11]  Jennifer Southgate,et al.  The relationship between the mechanical properties and cell behaviour on PLGA and PCL scaffolds for bladder tissue engineering. , 2009, Biomaterials.

[12]  A. Elmustafa Pile-up/sink-in of rate-sensitive nanoindentation creeping solids , 2007 .

[13]  E. Rabkin,et al.  On the nature of displacement bursts during nanoindentation of ultrathin Ni films on sapphire , 2010 .

[14]  I. Gutiérrez,et al.  Correlation between nanoindentation and tensile properties influence of the indentation size effect , 2003 .

[15]  R. Ramírez-Bon,et al.  Determination of fracture toughness and energy dissipation of SiO2-poly(methyl metacrylate) hybrid films by nanoindentation , 2011 .

[16]  J. Southgate,et al.  Influence of the physical properties of two-dimensional polyester substrates on the growth of normal human urothelial and urinary smooth muscle cells in vitro. , 2007, Biomaterials.

[17]  M. Oubaha,et al.  Corrosion protection of AA 2024-T3 aluminium alloys using 3, 4-diaminobenzoic acid chelated zirconium-silane hybrid sol-gels , 2010 .

[18]  B. Bergman,et al.  Method to account for true contact area in soda-lime glass during nanoindentation with the Berkovich tip , 2005 .

[19]  Saulius Juodkazis,et al.  Three-dimensional microfabrication of materials by femtosecond lasers for photonics applications , 2009 .

[20]  J. Vlassak,et al.  Determination of indenter tip geometry and indentation contact area for depth-sensing indentation experiments , 1998 .

[21]  Renzo M. Paulus,et al.  Tunable pH- and Temperature-Sensitive Copolymer Libraries by Reversible Addition−Fragmentation Chain Transfer Copolymerizations of Methacrylates , 2007 .

[22]  H. Jennissen,et al.  Peri-implant reactivity and osteoinductive potential of immobilized rhBMP-2 on titanium carriers. , 2010, Acta biomaterialia.

[23]  M. P. Gómez,et al.  Relation between the scratch resistance and the chemical structure of organic–inorganic hybrid coatings , 2011 .

[24]  Shiro Biwa,et al.  An analysis of fully plastic Brinell indentation , 1995 .

[25]  Alexei Bolshakov,et al.  Influences of stress on the measurement of mechanical properties using nanoindentation: Part II. Finite element simulations , 1996 .

[26]  Pedro Gómez-Romero,et al.  Functional Hybrid Materials , 2004 .

[27]  Yang-Tse Cheng,et al.  Relationships between hardness, elastic modulus, and the work of indentation , 1998 .

[28]  Huajian Gao,et al.  Indentation size effects in crystalline materials: A law for strain gradient plasticity , 1998 .

[29]  Capucine Sassoye,et al.  “Chimie douce”: A land of opportunities for the designed construction of functional inorganic and hybrid organic-inorganic nanomaterials , 2010, Comptes Rendus Chimie.

[30]  C. Charitidis,et al.  Nanomechanical and nanotribological properties of carbon-based thin films: A review , 2010 .

[31]  George M. Pharr,et al.  Influences of stress on the measurement of mechanical properties using nanoindentation: Part I. Experimental studies in an aluminum alloy , 1996 .

[32]  M. Swain,et al.  Determination of fracture toughness from the extra penetration produced by indentation-induced pop-in , 2003 .

[33]  B. Fabes,et al.  Mechanical properties of sol-gel coatings , 1990 .

[34]  Douglas A. Loy,et al.  Bridged Polysilsesquioxanes. Highly Porous Hybrid Organic‐Inorganic Materials , 1995 .

[35]  Clément Sanchez,et al.  Sol-gel chemistry of transition metal oxides , 1988 .

[36]  A. Zdunek,et al.  A theoretical study of the Brinell hardness test , 1989, Proceedings of the Royal Society of London. A. Mathematical and Physical Sciences.

[37]  C. Charitidis,et al.  Pre-osteoblastic cell response on three-dimensional, organic-inorganic hybrid material scaffolds for bone tissue engineering. , 2013, Journal of biomedical materials research. Part A.

[38]  D. Tabor Hardness of Metals , 1937, Nature.

[39]  Per Freiesleben Hansen,et al.  Water-entrained cement-based materials , 2001 .

[40]  Renata Reisfeld,et al.  The nature of the silica cage as reflected by spectral changes and enhanced photostability of trapped Rhodamine 6G , 1984 .

[41]  William D. Nix,et al.  Effects of the substrate on the determination of thin film mechanical properties by nanoindentation , 2002 .

[42]  G. Pharr,et al.  An improved technique for determining hardness and elastic modulus using load and displacement sensing indentation experiments , 1992 .

[43]  R. Corriu Les matériaux hybrides monophases organique-inorganique , 1998 .

[44]  J. Barbera,et al.  Contact mechanics , 1999 .

[45]  L. Dong,et al.  A novel approach for preparation of pH-sensitive hydrogels for enteric drug delivery , 1991 .

[46]  C. R. Becer,et al.  Water uptake of hydrophilic polymers determined by a thermal gravimetric analyzer with a controlled humidity chamber , 2007 .

[47]  A Ranella,et al.  Direct laser writing of 3D scaffolds for neural tissue engineering applications , 2011, Biofabrication.

[48]  William D. Nix,et al.  A method for interpreting the data from depth-sensing indentation instruments , 1986 .

[49]  J. Georges,et al.  Vickers Indentation Curves of Magnesium Oxide (MgO) , 1984 .

[50]  P. Bowen,et al.  Changes in portlandite morphology with solvent composition: Atomistic simulations and experiment , 2011 .

[51]  A. C. Fischer-Cripps,et al.  A simple phenomenological approach to nanoindentation creep , 2004 .

[52]  William D. Nix,et al.  Soft films on hard substrates — nanoindentation of tungsten films on sapphire substrates , 2001 .

[53]  R. King,et al.  Elastic analysis of some punch problems for a layered medium , 1987 .

[54]  A. Duri,et al.  Fracture study of organic–inorganic coatings using nanoindentation technique , 2004 .

[55]  Zhuangde Jiang,et al.  Investigation on methods for dealing with pile-up errors in evaluating the mechanical properties of thin metal films at sub-micron scale on hard substrates by nanoindentation technique , 2008 .

[56]  Paolo Colombo,et al.  Swelling-controlled release in hydrogel matrices for oral route , 1993 .

[57]  Subra Suresh,et al.  DETERMINATION OF ELASTOPLASTIC PROPERTIES BY INSTRUMENTED SHARP INDENTATION , 1999 .

[58]  L. Edwards,et al.  A combined experimental and finite element approach for determining mechanical properties of aluminium alloys by nanoindentation , 2010 .

[59]  C. Sanchez,et al.  DESIGN OF HYBRID ORGANIC-INORGANIC MATERIALS SYNTHESIZED VIA SOL-GEL CHEMISTRY , 1994 .

[60]  M. Popall,et al.  Applications of hybrid organic–inorganic nanocomposites , 2005 .

[61]  Valérie Cabuil,et al.  Designed Hybrid Organic−Inorganic Nanocomposites from Functional Nanobuilding Blocks , 2001 .

[62]  S. Calas-Etienne,et al.  Relation between structure and mechanical properties (elastoplastic and fracture behavior) of hybrid organic–inorganic coating , 2009 .

[63]  A. E. H. Love,et al.  BOUSSINESQ'S PROBLEM FOR A RIGID CONE , 1939 .

[64]  Lisa C. Klein,et al.  Sol-Gel Technology for Thin Films, Fibers, Preforms, Electronics and Specialty Shapes , 1988 .

[65]  C. Fotakis,et al.  Diffusion-assisted high-resolution direct femtosecond laser writing. , 2012, ACS nano.

[66]  G. Pharr,et al.  Influence of indenter tip geometry on elastic deformation during nanoindentation. , 2005, Physical review letters.

[67]  C. Brinker,et al.  Sol-Gel Science: The Physics and Chemistry of Sol-Gel Processing , 1990 .

[68]  O. Soppera,et al.  Mechanical properties of UV-photopolymerizable hybrid sol–gel films investigated by AFM in Pulsed Force Mode , 2005 .

[69]  Growth and bonding structure of hard hydrogenated amorphous carbon thin films deposited from an electron cyclotron resonance plasma , 2002 .

[70]  R. Sempéré,et al.  Mechanical properties of nanocomposite organosilicate films , 1998 .