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      Multi-functional nano-adhesive releasing therapeutic ions for MMP-deactivation and remineralization

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          Abstract

          Restoration of hard tissue in conjunction with adhesive is a globally challenging issue in medicine and dentistry. Common clinical therapies involving application of adhesive and substitute material for functional or anatomical recovery are still suboptimal. Biomaterials with bioactivity and inhibitory effects of enzyme-mediated adhesive degradation can render a solution to this. Here, we designed a novel copper-doped bioactive glass nanoparticles (CuBGn) to offer multifunction: metalloproteinases (MMP) deactivation and remineralization and incorporated the CuBGn in resin-dentin adhesive systems, which showed most common failure of MMP mediated adhesive degradation among hard tissue adhesives, to evaluate proposed therapeutic effects. A sol-gel derived bioactive glass nanoparticles doping 10 wt% of Cu (Cu-BGn) for releasing Cu ions, which were well-known MMP deactivator, were successfully created and included in light-curing dental adhesive (DA), a filler-free co-monomer resin blend, at different concentrations (up to 2 wt%). These therapeutic adhesives (CuBGn-DA) showed enhanced (a)cellular bioactivity, cytocompatibility, microtensile bond strength and MMP deactivation-ability. In conclusion, the incorporation of Cu ions releasing nano-bioactive glass demonstrated multifunctional properties at the resin-dentin interface; MMP deactivation and remineralization, representing a suitable strategy to extend the longevity of adhesive-hard tissue (i.e. resin-dentin) interfaces.

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          Most cited references37

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          Comparison of nanoscale and microscale bioactive glass on the properties of P(3HB)/Bioglass composites.

          This study compares the effects of introducing micro (m-BG) and nanoscale (n-BG) bioactive glass particles on the various properties (thermal, mechanical and microstructural) of poly(3hydroxybutyrate) (P(3HB))/bioactive glass composite systems. P(3HB)/bioactive glass composite films with three different concentrations of m-BG and n-BG (10, 20 and 30 wt%, respectively) were prepared by a solvent casting technique. The addition of n-BG particles had a significant stiffening effect on the composites, modulus when compared with m-BG. However, there were no significant differences in the thermal properties of the composites due to the addition of n-BG and m-BG particles. The systematic addition of n-BG particles induced a nanostructured topography on the surface of the composites, which was not visible by SEM in m-BG composites. This surface effect induced by n-BG particles considerably improved the total protein adsorption on the n-BG composites compared to the unfilled polymer and the m-BG composites. A short term in vitro degradation (30 days) study in simulated body fluid (SBF) showed a high level of bioactivity as well as higher water absorption for the P(3HB)/n-BG composites. Furthermore, a cell proliferation study using MG-63 cells demonstrated the good biocompatibility of both types of P(3HB)/bioactive glass composite systems. The results of this investigation confirm that the addition of nanosized bioactive glass particles had a more significant effect on the mechanical and structural properties of a composite system in comparison with microparticles, as well as enhancing protein adsorption, two desirable effects for the application of the composites in tissue engineering.
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            Reactivation of inactivated endogenous proteolytic activities in phosphoric acid-etched dentine by etch-and-rinse adhesives.

            Auto-degradation of collagen matrices occurs in resin-infiltrated dentine by the slow action of host-derived matrix metalloproteinases. As phosphoric acid-etching inactivates these endogenous enzymes, it is puzzling how hybrid layers created by simplified etch-and-rinse adhesives can degrade in vivo. This study tested the null hypothesis that there are no differences in the relative proteolytic activities of mineralised dentine, acid-etched dentine, and etch-and-rinse adhesive-treated acid-etched dentine. Powdered dentine prepared from extracted human teeth was treated with 17% EDTA, 10% phosphoric acid, or with five simplified etch-and-rinse adhesives that were applied to 10% phosphoric acid-etched dentine. The gelatinolytic activity of the dentine powder was assayed using fluorescein-labelled gelatine. TEM examination of the air-dried, treated dentine powder was performed to confirm the presence of remnant mineralised dentine after acid-etching. 17% EDTA significantly reduced the relative proteolytic activity (73.2%) of the untreated mineralised dentine powder (control), while 10% phosphoric acid-etched dentine exhibited the highest reduction (98.1%). Treating the acid-etched dentine powder with any of the five simplified etch-and-rinse adhesives resulted in the reactivation of the proteolytic activity, with a significant negative linear correlation (P<0.05) between the increases in fluorescence and the corresponding pH values of the adhesives. It is concluded that simplified etch-and-rinse adhesives can reactivate endogenous enzymatic activities in dentine that are previously inactivated by phosphoric acid-etching. The amount of enzyme reactivated may even exceed the original quantity present in untreated mineralised dentine. This provides an explanation for the degradation of hybrid layers after acid-etched dentine matrices are infiltrated with these adhesives.
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              MMP Inhibitors on Dentin Stability: A Systematic Review and Meta-analysis.

              The aim of this study was to systematically review the literature for in vitro and ex vivo studies that evaluated the effect of matrix metalloproteinase (MMP) inhibitors during the adhesive procedure on the immediate and long-term resin-dentin bond strength. The search was conducted in 6 databases with no publication year or language limits, following the Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) statement. From 1,336 potentially eligible studies, 48 were selected for full-text analysis, and 30 were included for review, with 17 considered in the meta-analysis. Two reviewers independently selected the studies, extracted the data, and assessed the risk of bias. Pooled effect estimates were expressed as the weighted mean difference between groups. The most used MMP inhibitor was chlorhexidine (CHX). Immediate bond strength results showed no difference between 2% CHX and control; however, a difference was found between 0.2% CHX and control at baseline. After aging, CHX presented higher bond strength values compared to control groups (p < .05). However, this was not observed for longer periods of aging. High heterogeneity was found in some comparisons, especially for the water storage aging subgroup. Subgroup analyses showed that self-etching and etch-and-rinse adhesives are benefited by the CHX use. From the studies included, only 1 presented low risk of bias, while the others showed medium or high risk of bias. The use of MMP inhibitors did not affect the immediate bond strength overall, while it influenced the aged bond strength. Aging procedures influenced bond strength values of the dentin adhesion stability.
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                Author and article information

                Contributors
                ducious@gmail.com
                haelee@dku.edu
                Journal
                Sci Rep
                Sci Rep
                Scientific Reports
                Nature Publishing Group UK (London )
                2045-2322
                4 April 2018
                4 April 2018
                2018
                : 8
                : 5663
                Affiliations
                [1 ]ISNI 0000 0004 4672 1057, GRID grid.443780.c, Department of Dental Hygiene, , Kyungdong University, ; Wonju 26495, South Korea
                [2 ]ISNI 0000 0001 0705 4288, GRID grid.411982.7, Department of Biomaterials Science, , School of Dentistry, Dankook University, ; Cheonan 31116, South Korea
                [3 ]ISNI 0000 0001 0705 4288, GRID grid.411982.7, Institute of Tissue Regeneration Engineering (ITREN), , Dankook University, ; Cheonan, 31116 South Korea
                [4 ]ISNI 0000 0004 0432 6841, GRID grid.45083.3a, Lithuanian University of health sciences, ; Kaunas, 44307 Lithuania
                [5 ]ISNI 0000 0001 2151 8157, GRID grid.419725.c, Glass Research Department, , National Research centre, ; Cairo, 12622 Egypt
                [6 ]ISNI 0000 0001 2171 7818, GRID grid.289247.2, Department of Conservative Dentistry, , School of Dentistry, Kyung Hee University, ; 02447 Seoul, South Korea
                [7 ]ISNI 0000 0004 0470 5454, GRID grid.15444.30, Department of Dental Hygiene, , Yonsei University Wonju College of Medicine, ; Wonju, 26426 South Korea
                [8 ]ISNI 0000 0004 1769 4352, GRID grid.412878.0, Dental Biomaterials, Departamento de Odontología, , Facultad de Ciencias de la Salud, University CEU-Cardenal Herrera, ; Valencia, Spain
                [9 ]ISNI 0000 0001 2322 6764, GRID grid.13097.3c, Tissue Engineering & Biophotonics, , King’s College London Dental Institute (KCLDI), ; London, UK
                [10 ]ISNI 0000 0001 0705 4288, GRID grid.411982.7, Department of Nanobiomedical Science & BK21 PLUS NBM Global Research Center for Regenerative Medicine Research Center, , Dankook University, ; Cheonan, 31116 South Korea
                Author information
                http://orcid.org/0000-0002-7204-7102
                http://orcid.org/0000-0002-2527-8776
                http://orcid.org/0000-0001-8678-5459
                http://orcid.org/0000-0001-7224-5507
                Article
                23939
                10.1038/s41598-018-23939-6
                5884793
                29618810
                81c7ff30-9883-4dac-9d40-8f4b6fd3ccc0
                © The Author(s) 2018

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 13 November 2017
                : 23 March 2018
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