Modified POSS nano-structures as novel co-initiator-crosslinker: Synthesis and characterization

Abstract

Objective: To synthesize an amine-modified polyhedral oligomeric silsesquioxane (POSS) nano-structure as a novel co-initiator-crosslinker (co-Ini-Linker) and to determine the effect of the co-Ini-linker on the physical and mechanical behavior of an experimental dental composite.

Methods: The amine-methacrylate POSS nano-structures (AMA-POSS) were chemically synthesized by anchoring a tertiary amine functionality on the methacrylate POSS (MA-POSS) branches. Three types of AMA-POSS, having different amine branches in their structures, were synthesized through the Aza Michael reaction. The chemical structure of AMA-POSSs were evaluated by¹H-NMR spectroscopy. Afterward, the AMA-POSS was incorporated into a dental resin system composed of Bis-GMA, TEGDMA, and photo-initiator. Three resin systems with different AMA-POSS types were then prepared, and their properties were compared with a resin containing DMAEMA as a conventional co-initiator. The degree of conversion evaluated by FTIR spectroscopy and the shrinkage kinetics of the resins were determined through the bonded-disk technique. The flexural properties of the photopolymerized resins were also investigated. The distribution of nano-structures in the matrix resin was analyzed using EDX analysis.

Results: The modified POSS structure and the number of amine branches were confirmed with¹H-NMR spectroscopy. The resin containing 8 amine branches (P8) showed the same degree of conversion (DC%) as the resin containing DMAEMA (P > 0.05). Decreasing the amine branches in the POSS structure, however, revealed an increasing trend in DC%. The resin containing P8 showed the lowest shrinkage strain. By incorporating AMA-POSS into the resin system, the water sorption significantly decreased (P < 0.05). The flexural strength and modulus increased by adding P3 into the resin system (P < 0.05). EDX Si-map revealed that the co-Ini-linker was well dispersed in the resin matrix.

Significance: The synthesized novel amine-methacrylate POSS nanostructures not only act as an amine co-initiator but also work as a reinforcing filler and a cross-linking agent.

Keywords: Co-Initiator; Crosslinker; Dental resins; POSS; Photo-Initiator.