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Directed Mineralization on Polyelectrolyte Multilayer Films

Published online by Cambridge University Press:  26 February 2011

Maria C. Advincula ,
Pritesh A. Patel ,
Patrick T. Mather ,
Daniel Underhill ,
Bryan D. Huey  and
A. Jon Goldberg
Maria C. Advincula
Affiliation:
madvincula@uchc.edu, University of Connecticut Health Center, Oral Rehabilitation, 263 Farmington Ave, MC-1615, Farmington CT 06030United States
Pritesh A. Patel
Affiliation:
pritesh.patel@case.edu, Case Western Reserve University, Macromolecular Science and Engineering, 312 Kent Hale Smith Building, 2100 Adelbert Road, Cleveland, OH, 44106, United States
Patrick T. Mather
Affiliation:
patrick.mather@case.edu, Case Western Reserve University, Macromolecular Science and Engineering, 312 Kent Hale Smith Building, 2100 Adelbert Road, Cleveland, OH, 44106, United States
Daniel Underhill
Affiliation:
Pyfll@yahoo.com, University of Connecticut, Institute of Materials Science, 97 North Eagleville Road, Storrs, CT, 06269, United States
Bryan D. Huey
Affiliation:
bhuey@ims.uconn.edu, University of Connecticut, Institute of Materials Science, 97 North Eagleville Road, Storrs, CT, 06269, United States
A. Jon Goldberg
Affiliation:
goldberg@uchc.edu, University of Connecticut Health Center, Oral Rehabilitation, 263 Farmington Ave, MC-1615, Farmington, CT, 06030, United States
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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 where in 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.

Keywords

Sicatalyticbiomimetic (chemical reaction)
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 975: Symposium DD – Mechanics of Biological and Bio-Inspired Materials , 2006 , 0975-DD06-03
Copyright
Copyright © Materials Research Society 2007

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References

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