Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance
The leading cause of composite restoration failure is recurrent marginal decay. The margin between the composite and tooth is initially sealed by a low-viscosity adhesive, but chemical, physical, and mechanical stresses work synergistically and simultaneously to degrade the adhesive, destroying the...
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Frontiers Media S.A.
2024-04-01
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| Series: | Frontiers in Dental Medicine |
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| Online Access: | https://www.frontiersin.org/articles/10.3389/fdmed.2024.1373853/full |
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| author | Burak Korkmaz Erhan Demirel Qiang Ye Qiang Ye Anil Misra Anil Misra Candan Tamerler Candan Tamerler Candan Tamerler Paulette Spencer Paulette Spencer Paulette Spencer |
| author_facet | Burak Korkmaz Erhan Demirel Qiang Ye Qiang Ye Anil Misra Anil Misra Candan Tamerler Candan Tamerler Candan Tamerler Paulette Spencer Paulette Spencer Paulette Spencer |
| author_sort | Burak Korkmaz |
| collection | DOAJ |
| description | The leading cause of composite restoration failure is recurrent marginal decay. The margin between the composite and tooth is initially sealed by a low-viscosity adhesive, but chemical, physical, and mechanical stresses work synergistically and simultaneously to degrade the adhesive, destroying the interfacial seal and providing an ideal environment for bacteria to proliferate. Our group has been developing self-strengthening adhesives with improved chemical and mechanical characteristics. This paper reports a self-strengthening adhesive formulation that resists hydrolysis-mediated degradation by providing intrinsic reinforcement of the polymer network through synergistic stimulation of free-radical polymerization, sol-gel reaction, and hydrophobicity. Hydrophobic resin formulation (NE1) was developed using HEMA/BisGMA 28/55w/w and 15 wt% MPS. Control (NC1) contained HEMA/BisGMA 28/55 w/w and 15 wt% MES. The polymerization kinetics, water sorption, leachates, and dynamic mechanical properties of the resin samples were investigated. The NC1 and NE1 samples showed comparable polymerization kinetics, degrees of conversion and water sorption. In contrast, NC1 showed significantly higher levels of HEMA and BisGMA leachate, indicating faster degradation in ethanol. At day 3, cumulative HEMA leachate for NC1 was ten times greater than NE1 (p < 0.05). Dynamic mechanical properties were measured at 37 and 70°C in both dry and wet conditions. Under dry conditions, the storage moduli of NC1 and NE1 were comparable and the glass transition temperature (Tg) of NC1 was statistically significantly lower (p < 0.001) than NE1. Under wet conditions, the storage modulus of NC1 was lower than NE1 and at 70°C there was a threefold difference in storage modulus. At this temperature and under wet conditions, the storage modulus of NC1 is statistically significantly lower (p < 0.001) than NE1. The results indicated that in the wet environment, NE1 provided lower chain mobility, higher crosslink density, and more hydrogen bonds. The newly formulated methacrylate-based adhesive capitalizes on free-radical polymerization, sol-gel reactions, and hydrophobicity to provide enhanced mechanical properties at elevated temperatures in wet environments and hydrolytic stability under aggressive aging conditions. |
| format | Article |
| id | doaj-art-61827bc2928a4a53b9e5560df240f9b7 |
| institution | Kabale University |
| issn | 2673-4915 |
| language | English |
| publishDate | 2024-04-01 |
| publisher | Frontiers Media S.A. |
| record_format | Article |
| series | Frontiers in Dental Medicine |
| spelling | doaj-art-61827bc2928a4a53b9e5560df240f9b72025-02-11T10:53:38ZengFrontiers Media S.A.Frontiers in Dental Medicine2673-49152024-04-01510.3389/fdmed.2024.13738531373853Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistanceBurak Korkmaz0Erhan Demirel1Qiang Ye2Qiang Ye3Anil Misra4Anil Misra5Candan Tamerler6Candan Tamerler7Candan Tamerler8Paulette Spencer9Paulette Spencer10Paulette Spencer11Institute for Bioengineering Research, University of Kansas, Lawrence, KS, United StatesInstitute for Bioengineering Research, University of Kansas, Lawrence, KS, United StatesInstitute for Bioengineering Research, University of Kansas, Lawrence, KS, United StatesCanon Virginia, Inc., Newport News, VA, United StatesInstitute for Bioengineering Research, University of Kansas, Lawrence, KS, United StatesDepartment of Civil and Environmental Engineering, Florida International University, Miami, FL, United StatesInstitute for Bioengineering Research, University of Kansas, Lawrence, KS, United StatesDepartment of Mechanical Engineering, University of Kansas, Lawrence, KS, United StatesBioengineering Program, University of Kansas, Lawrence, KS, United StatesInstitute for Bioengineering Research, University of Kansas, Lawrence, KS, United StatesDepartment of Mechanical Engineering, University of Kansas, Lawrence, KS, United StatesBioengineering Program, University of Kansas, Lawrence, KS, United StatesThe leading cause of composite restoration failure is recurrent marginal decay. The margin between the composite and tooth is initially sealed by a low-viscosity adhesive, but chemical, physical, and mechanical stresses work synergistically and simultaneously to degrade the adhesive, destroying the interfacial seal and providing an ideal environment for bacteria to proliferate. Our group has been developing self-strengthening adhesives with improved chemical and mechanical characteristics. This paper reports a self-strengthening adhesive formulation that resists hydrolysis-mediated degradation by providing intrinsic reinforcement of the polymer network through synergistic stimulation of free-radical polymerization, sol-gel reaction, and hydrophobicity. Hydrophobic resin formulation (NE1) was developed using HEMA/BisGMA 28/55w/w and 15 wt% MPS. Control (NC1) contained HEMA/BisGMA 28/55 w/w and 15 wt% MES. The polymerization kinetics, water sorption, leachates, and dynamic mechanical properties of the resin samples were investigated. The NC1 and NE1 samples showed comparable polymerization kinetics, degrees of conversion and water sorption. In contrast, NC1 showed significantly higher levels of HEMA and BisGMA leachate, indicating faster degradation in ethanol. At day 3, cumulative HEMA leachate for NC1 was ten times greater than NE1 (p < 0.05). Dynamic mechanical properties were measured at 37 and 70°C in both dry and wet conditions. Under dry conditions, the storage moduli of NC1 and NE1 were comparable and the glass transition temperature (Tg) of NC1 was statistically significantly lower (p < 0.001) than NE1. Under wet conditions, the storage modulus of NC1 was lower than NE1 and at 70°C there was a threefold difference in storage modulus. At this temperature and under wet conditions, the storage modulus of NC1 is statistically significantly lower (p < 0.001) than NE1. The results indicated that in the wet environment, NE1 provided lower chain mobility, higher crosslink density, and more hydrogen bonds. The newly formulated methacrylate-based adhesive capitalizes on free-radical polymerization, sol-gel reactions, and hydrophobicity to provide enhanced mechanical properties at elevated temperatures in wet environments and hydrolytic stability under aggressive aging conditions.https://www.frontiersin.org/articles/10.3389/fdmed.2024.1373853/fulldental adhesivehydrolytic degradationhighly crosslinked networksol-gel reactiondynamic mechanical analysishydrophobic resins |
| spellingShingle | Burak Korkmaz Erhan Demirel Qiang Ye Qiang Ye Anil Misra Anil Misra Candan Tamerler Candan Tamerler Candan Tamerler Paulette Spencer Paulette Spencer Paulette Spencer Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance Frontiers in Dental Medicine dental adhesive hydrolytic degradation highly crosslinked network sol-gel reaction dynamic mechanical analysis hydrophobic resins |
| title | Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance |
| title_full | Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance |
| title_fullStr | Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance |
| title_full_unstemmed | Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance |
| title_short | Synergistic enhancement of hydrophobic dental adhesives: autonomous strengthening, polymerization kinetics, and hydrolytic resistance |
| title_sort | synergistic enhancement of hydrophobic dental adhesives autonomous strengthening polymerization kinetics and hydrolytic resistance |
| topic | dental adhesive hydrolytic degradation highly crosslinked network sol-gel reaction dynamic mechanical analysis hydrophobic resins |
| url | https://www.frontiersin.org/articles/10.3389/fdmed.2024.1373853/full |
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