Viscoelastic properties of collagen–adhesive composites under water‐saturated and dry conditions

et al. 2016

Acta Biomaterialia

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Chemical and enzymatic hydrolysis provoke a cascade of events that undermine methacrylate-based adhesives and the bond formed at the tooth/composite interface. Infiltration of noxious agents, e.g. enzymes, bacteria, and so forth, into the spaces created by the defective bond will ultimately lead to failure of the composite restoration. This paper reports a novel, synthetic resin that provides enhanced hydrolytic stability as a result of intrinsic reinforcement of the polymer network. The behavior of this novel resin, which contains γ-methacryloxyproyl trimethoxysilane (MPS) as its Si-based compound, is reminiscent of self-strengthening properties found in nature. The efforts in this paper are focused on two essential aspects: the visible-light irradiation induced (photoacid-induced) sol-gel reaction and the mechanism leading to intrinsic self-strengthening. The FTIR band at 2840 cm−1 corresponding to CH3 symmetric stretch in −Si−O−CH3 was used to evaluate the sol-gel reaction. Results from the real-time FTIR indicated that the newly developed resin showed a limited sol-gel reaction (<5%) during visible-light irradiation, but after 48h dark storage, the reaction was over 65%. The condensation of methoxysilane mainly occurred under wet conditions. The storage moduli and glass transition temperature of the copolymers increased in wet conditions with the increasing MPS content. The cumulative amounts of leached species decreased significantly when the MPS-containing adhesive was used. The results suggest that the polymethacrylate-based network, which formed first as a result of free radical initiated polymerization, retarded the photoacid-induced sol-gel reaction. The sol-gel reaction provided a persistent, intrinsic reinforcement of the polymer network in both neutral and acidic conditions. This behavior led to enhanced mechanical properties of the dental adhesives under conditions that simulate the wet, oral environment.

Section: Discussionmentioning

confidence: 99%

Mimicking nature: Self-strengthening properties in a dental adhesive

et al. 2016

Acta Biomaterialia

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“…Simultaneous water diffusion and mechanical loading can lead to anomalously high creep strain or lower strength in some polymers. 58,59 Using EDMAB as a coinitiator, the modulus of the hybrid formulations with ES-4 content up to 35% was significantly higher than that of the control (C0-EDMAB, p < 0.05) at 70°C. This means that with the increase in ES-4 content, the highly crosslinked structure can counteract the effect of water plasticization.…”

Section: Discussionmentioning

confidence: 89%

Development of methacrylate/silorane hybrid monomer system: Relationship between photopolymerization behavior and dynamic mechanical properties

et al. 2015

J Biomed Mater Res

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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.

“…Neglecting this important parameter hampers the development of clinically durable dental adhesives. For example, investigators showed that time- and rate-dependent behavior can have a profound effect on stress concentration at the dentin/adhesive (d/a) interface [ 18 , 19 , 20 ] and failure at the d/a interface is determined by the component whose stress concentration is closest to its failure strength [ 19 , 20 , 21 , 22 , 23 ].…”

Section: Introductionmentioning

confidence: 99%

Evolution of Network Structure and Mechanical Properties in Autonomous-Strengthening Dental Adhesive

Sarikaya

et al. 2020

Polymers

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The inherent degradation property of most dental resins in the mouth leads to the long-term release of degradation by-products at the adhesive/tooth interface. The by-products increase the virulence of cariogenic bacteria, provoking a degradative positive-feedback loop that leads to physicochemical and mechanical failure. Photoinduced free-radical polymerization and sol‒gel reactions have been coupled to produce a novel autonomous-strengthening adhesive with enhanced hydrolytic stability. This paper investigates the effect of network structure on time-dependent mechanical properties in adhesives with and without autonomous strengthening. Stress relaxation was conducted under 0.2% strain for 8 h followed by 40 h recovery in water. The stress‒time relationship is analyzed by nonlinear least-squares data-fitting. The fitted Prony series predicts the sample’s history under monotonic loading. Results showed that the control failed after the first loading‒unloading‒recovery cycle with permanent deformation. While for the experimental sample, the displacement was almost completely recovered and the Young’s modulus increased significantly after the first test cycle. The experimental polymer exhibited higher degree of conversion, lower leachate, and time-dependent stiffening characteristics. The autonomous-strengthening reaction persists in the aqueous environment leading to a network with enhanced resistance to deformation. The results illustrate a rational approach for tuning the viscoelasticity of durable dental adhesives.