Modification of filler surface treatment of composite resins using alternative silanes and functional nanogels

Abstract

Objectives: This study probes how modifiedapproaches for filler surface treatment in dental composites based on alternative silanes and functional nanogel additives affects physicochemical properties of these materials with a focus on polymerization stress development.

Methods: Nanogels were synthesized from isobornyl methacrylate, ethoxylated bisphenol-A dimethacrylate and isocyanatoethyl methacrylate followed by partial further reaction with 2-hydroxyethyl methacrylate to provide both isocyanate and methacrylate functionalization. A barium glass filler (˜1 μm particle size) was treated with either γ-methacryloxypropyltrimethoxysilane (MPS), N-methylaminopropyltrimethoxy (MAP) or N-allylaminopropyltrimethoxy (AAP) silanes. The reactive nanogels were then covalently attached to the aminosilane-treated fillers. Surface treatment was characterized by thermogravimetric analysis (TGA) and diffuse reflectance infrared spectroscopy (DR-IR). Composites were formulated with 60 wt% of the various functionalized fillers and the materials were evaluated for polymerization kinetics, polymerization stress (PS), volumetric shrinkage, mechanical properties and photorheology. Data were evaluated by one-way ANOVA and Tukey's test at 5% significance level.

Results: Filler surface treatments were confirmed by TGA and DR-IR analyses. Nanogel-functionalized fillers significantly reduced PS up to 20%, while the degree of conversion and elastic modulus were not compromised. Similar storage modulus development during polymerization was observed among materials by photorheology although the rate of polymerization was significantly increased for nanogel-based treatments. A significant decrease in flexural strength was observed for amino functional silane groups; however, there was no statistical difference in strength for the MPS control group compared with the nanogel-modified composites.

Significance: Filler surface treatment modified with a reactive nanogel enables significant PS reduction, without compromise to degree of conversion or mechanical properties of dental composites.

Keywords: Composite resin; Fillers; Isocyanates; Mechanical properties; Methacrylates; Nanogels; Polymerization; Silanization; Stress; Surface treatment.