Development of methacrylate/silorane hybrid monomer system: Relationship between photopolymerization behavior and dynamic mechanical properties
Laurence, Jennifer S.
Berrie, Cindy L.
Scholarly/refereed, author accepted manuscript
This is the peer reviewed version of the following article: Song, L., Ye, Q., Ge, X., Singh, V., Misra, A., Laurence, J. S., … Spencer, P. (2016). Development of methacrylate/silorane hybrid monomer system: Relationship between photopolymerization behavior and dynamic mechanical properties. Journal of Biomedical Materials Research. Part B, Applied Biomaterials, 104(5), 841–852. http://doi.org/10.1002/jbm.b.33435, which has been published in final form at 10.1002/jbm.b.33435. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.
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Resin chemistries for dental composite are evolving as noted by the introduction of silorane-based composites in 2007. This shift in the landscape from methacrylate-based composites has fueled the quest for versatile methacrylate-silorane adhesives. The objective of this study was to evaluate the polymerization behavior and structure/property relationships of methacrylate-silorane hybrid systems. Amine compound ethyl-4-(dimethylamino) benzoate (EDMAB) or silane compound tris(trimethylsilyl) silane (TTMSS) was selected as coinitiators. The mechanical properties of the copolymer were improved significantly at low concentrations (15, 25, or 35 wt %) of silorane when EDMAB was used as coinitiator. The rubbery moduli of these experimental copolymers were increased by up to 260%, compared with that of the control (30.8 ± 1.9 MPa). Visible phase separation appeared in these formulations if the silorane concentrations in the formulations were 50–75 wt %. The use of TTMSS as coinitiator decreased the phase separation, but there was a concomitant decrease in mechanical properties. In the neat methacrylate formulations, the maximum rates of free-radical polymerization with EDMAB or TTMSS were 0.28 or 0.06 s−1, respectively. In the neat silorane resin, the maximum rates of cationic ring-opening polymerization with EDMAB or TTMSS were 0.056 or 0.087 s−1, respectively. The phase separation phenomenon may be attributed to differences in the rates of free-radical polymerization of methacrylates and cationic ring-opening polymerization of silorane. In the hybrid systems, free-radical polymerization initiated with EDMAB led to higher crosslink density and better mechanical properties under dry/wet conditions. These beneficial effects were, however, associated with an increase in heterogeneity in the network structure.
Song, L., Ye, Q., Ge, X., Singh, V., Misra, A., Laurence, J. S., … Spencer, P. (2016). Development of methacrylate/silorane hybrid monomer system: Relationship between photopolymerization behavior and dynamic mechanical properties. Journal of Biomedical Materials Research. Part B, Applied Biomaterials, 104(5), 841–852. http://doi.org/10.1002/jbm.b.33435
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