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Reconfigurable Dual Peptide Tethered Polymer System Offers a Synergistic Solution for Next Generation Dental Adhesives.

ABSTRACT: Resin-based composite materials have been widely used in restorative dental materials due to their aesthetic, mechanical, and physical properties. However, they still encounter clinical shortcomings mainly due to recurrent decay that develops at the composite-tooth interface. The low-viscosity adhesive that bonds the composite to the tooth is intended to seal this interface, but the adhesive seal is inherently defective and readily damaged by acids, enzymes, and oral fluids. Bacteria infiltrate the resulting gaps at the composite-tooth interface and bacterial by-products demineralize the tooth and erode the adhesive. These activities lead to wider and deeper gaps that provide an ideal environment for bacteria to proliferate. This complex degradation process mediated by several biological and environmental factors damages the tooth, destroys the adhesive seal, and ultimately, leads to failure of the composite restoration. This paper describes a co-tethered dual peptide-polymer system to address composite-tooth interface vulnerability. The adhesive system incorporates an antimicrobial peptide to inhibit bacterial attack and a hydroxyapatite-binding peptide to promote remineralization of damaged tooth structure. A designer spacer sequence was incorporated into each peptide sequence to not only provide a conjugation site for methacrylate (MA) monomer but also to retain active peptide conformations and enhance the display of the peptides in the material. The resulting MA-antimicrobial peptides and MA-remineralization peptides were copolymerized into dental adhesives formulations. The results on the adhesive system composed of co-tethered peptides demonstrated both strong metabolic inhibition of S. mutans and localized calcium phosphate remineralization. Overall, the result offers a reconfigurable and tunable peptide-polymer hybrid system as next-generation adhesives to address composite-tooth interface vulnerability.

SUBMITTER: Yuca E

PROVIDER: S-EPMC8235192 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Dental adhesives are vital for the success of dental restorations. The objective of this study is to make strong and durable dental adhesives that are free from 2 symbolic methacrylate-based dental resins-2-bis[4-(2-hydroxy-3-methacryl-oxypropoxy)-phenyl]-propane (Bis-GMA) and 2-hydroxyethyl-methacrylate (HEMA)-and have equivalent/improved bonding strength and durability. We formulated, prepared, and evaluated 2 dental adhesives using mixtures of a hydrolytically stable ether-based monomer, triethylene glycol divinylbenzyl ether (TEG-DVBE), with urethane dimethacrylate (UDMA) or pyromellitic glycerol dimethacrylate. These adhesives were composed of equimolar ester-/ether-based vinyl functional groups. They were compared with Bis-GMA/HEMA-based commercial and experimental dental adhesives in terms of shear bond strength and microtensile bond strength (µTBS) to human dentin and the µTBS bond stability under extended thermocycling challenges. In addition, the resins' infiltration to dentin tubules, mechanical performance, and chemical properties were assessed by scanning electron microscopy, ISO standard flexural strength and modulus measurements, contact angle measurements, and water sorption/solubility measurements. The hybrid TEG-DVBE-containing dental adhesives generated equivalent shear bond strength and µTBS in comparison with the controls. Significantly, these adhesives outperformed the controls after being challenged by 10,000 thermocycles between 5 °C and 55 °C. Water contact angle measurements suggested that the hybrid dental adhesives were relatively more hydrophobic than the Bis-GMA/HEMA controls. However, both TEG-DVBE-containing adhesives developed more and deeper resin tags in dentin tubules and formed thicker hybrid layers at the composite-dentin interface. Furthermore, the water solubility of UDMA/TEG-DVBE resins was reduced approximately 89% in comparison with the Bis-GMA/HEMA controls. The relatively hydrophobic adhesives that achieved equivalent/enhanced bonding performance suggest great potentials in developing dental restoration with extended service life. Furthermore, the TEG-DVBE-containing materials may find wider dental applications and broader utility in medical device development.

Project description:Resin-based composite has overtaken dental amalgam as the most popular material for direct restorative dentistry. In spite of this popularity the clinical lifetime of composite restorations is threatened by recurrent decay. Degradation of the adhesive leads to gaps at the composite/tooth interface-bacteria, bacterial by-products and fluids infiltrate the gaps leading to recurrent decay and composite restoration failure. The durability of resin-dentin bonds is a major problem. We address this problem by synthesizing silyl-functionalized BisGMA (e.g., silyl-BisGMA), formulating dental adhesives with the new monomer and determining the physicochemical properties and leaching characteristics of the silyl-BisGMA adhesives. Silyl-BisGMA was synthesized by stoichiometric amounts of BisGMA and 3-isocyanatopropyl trimethoxysilane (IPTMS). The control adhesive was a mixture based on HEMA/BisGMA (45/55, w/w). In the experimental formulations, BisGMA was partially or completely replaced by silyl-BisGMA. Water miscibility, polymerization behavior (Fourier transform infrared spectroscopy, FTIR), thermal property (modulated differential scanning calorimetry, MDSC), mechanical properties in dry and wet conditions (dynamic mechanical analysis, DMA), and leached species (HPLC) were investigated. Data from all tests were submitted to appropriate statistical analysis (α = 0.05). Silyl-BisGMA-containing adhesives exhibited comparable water miscibility, lower viscosities, and significantly improved degree of conversion of CC bond as compared to the control. After 4 weeks aqueous aging, the glass transition temperature and rubbery moduli of the experimental copolymers were significantly greater than the control (p < 0.05). HPLC results indicated a substantial reduction of leached HEMA (up to 99 wt%) and BisGMA (up to 90 wt%). By introducing silyl-functional group, the new BisGMA derivative exhibited potential as a monomer that can lead to dental adhesives with improved mechanical properties and reduced leaching under conditions relevant to the oral environment. STATEMENT OF SIGNIFICANCE: The low-viscosity adhesive that bonds the composite to the tooth (enamel and dentin) is intended to seal and stabilize the composite/tooth interface, but it degrades leading to a breach at the composite/tooth margin. As the most popular crosslinking monomer in adhesives, Bisphenol A-glycerolate dimethacrylate (BisGMA) has limitations, e.g. susceptible to hydrolysis and concomitant property degradation. A methoxysilyl-functionalized BisGMA derivative (silyl-BisGMA) was introduced in this work to respond to these limitations. Our results indicated that by introducing silyl-BisGMA, higher crosslinked networks were obtained without sacrificing the homogeneity, and the leached amount of HEMA was reduced up to 99%. This novel resin offers potential benefits including prolonging the functional lifetime of dental resin materials.

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Reconfigurable Dual Peptide Tethered Polymer System Offers a Synergistic Solution for Next Generation Dental Adhesives.

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