Toughening and polymerization stress control in composites using thiourethane-treated fillers

Abstract Filler particle functionalization with thiourethane oligomers has been shown to increase fracture toughness and decrease polymerization stress in dental composites, though the mechanism is poorly understood. The aim of this study was to systematically characterize the effect of the type of...

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Main Authors: Ana Paula Piovezan Fugolin, Ana Rosa Costa, Lourenco Correr-Sobrinho, R. Crystal Chaw, Steven Lewis, Jack Liborio Ferracane, Carmem Silvia Pfeifer
Format: Article
Language:English
Published: Nature Portfolio 2021-04-01
Series:Scientific Reports
Online Access:https://doi.org/10.1038/s41598-021-87151-9
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author Ana Paula Piovezan Fugolin
Ana Rosa Costa
Lourenco Correr-Sobrinho
R. Crystal Chaw
Steven Lewis
Jack Liborio Ferracane
Carmem Silvia Pfeifer
author_facet Ana Paula Piovezan Fugolin
Ana Rosa Costa
Lourenco Correr-Sobrinho
R. Crystal Chaw
Steven Lewis
Jack Liborio Ferracane
Carmem Silvia Pfeifer
author_sort Ana Paula Piovezan Fugolin
collection DOAJ
description Abstract Filler particle functionalization with thiourethane oligomers has been shown to increase fracture toughness and decrease polymerization stress in dental composites, though the mechanism is poorly understood. The aim of this study was to systematically characterize the effect of the type of filler surface functionalization on the physicochemical properties of experimental resin composites containing fillers of different size and volume fraction. Barium glass fillers (1, 3 and 10 µm) were functionalized with 2 wt% thiourethane-silane (TU-Sil) synthesized de novo and characterized by thermogravimetric analysis. Fillers treated with 3-(Trimethoxysilyl)propyl methacrylate (MA-Sil) and with no surface treatment (No-Sil) served as controls. Fillers (50, 60 and 70 wt%) were incorporated into BisGMA-UDMA-TEGDMA (5:3:2) containing camphorquinone/ethyl-4-dimethylaminobenzoate (0.2/0.8 wt%) and 0.2 wt% di-tert-butyl hydroxytoluene. The functionalized particles were characterized by thermogravimetric analysis and a representative group was tagged with methacrylated rhodamine B and analyzed by confocal laser scanning microscopy. Polymerization kinetics were assessed by near-IR spectroscopy. Polymerization stress was tested in a cantilever system, and fracture toughness was assessed with single edge-notched beams. Fracture surfaces were characterized by SEM. Data were analyzed with ANOVA/Tukey's test (α = 0.05). The grafting of thiourethane oligomer onto the surface of the filler particles led to reductions in polymerization stress ranging between 41 and 54%, without affecting the viscosity of the composite. Fracture toughness increased on average by 35% for composites with the experimental fillers compared with the traditional methacrylate-silanized groups. SEM and confocal analyses demonstrate that the coverage of the filler surface was not homogeneous and varied with the size of the filler. The average silane layer for the 1 µm particle functionalized with the thiourethane was 206 nm, much thicker than reported for traditional silanes. In summary, this study systematically characterized the silane layer and established structure–property relationships for methacrylate and thiourethane silane-containing materials. The results demonstrate that significant stress reductions and fracture toughness increases are obtained by judiciously tailoring the organic–inorganic interface in dental composites.
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spelling doaj.art-6916197c59fe4ef48f370ddda361335f2022-12-21T20:39:05ZengNature PortfolioScientific Reports2045-23222021-04-0111111210.1038/s41598-021-87151-9Toughening and polymerization stress control in composites using thiourethane-treated fillersAna Paula Piovezan Fugolin0Ana Rosa Costa1Lourenco Correr-Sobrinho2R. Crystal Chaw3Steven Lewis4Jack Liborio Ferracane5Carmem Silvia Pfeifer6Division of Biomaterials and Biomechanics, Department of Restorative Dentistry, Oregon Health & Science UniversityDivision of Dental Materials, Department of Restorative Dentistry, Piracicaba Dental School—UNICAMPDivision of Dental Materials, Department of Restorative Dentistry, Piracicaba Dental School—UNICAMPAdvanced Light Microscopy Core, Department of Neurology, Oregon Health & Science UniversityDivision of Biomaterials and Biomechanics, Department of Restorative Dentistry, Oregon Health & Science UniversityDivision of Biomaterials and Biomechanics, Department of Restorative Dentistry, Oregon Health & Science UniversityDivision of Biomaterials and Biomechanics, Department of Restorative Dentistry, Oregon Health & Science UniversityAbstract Filler particle functionalization with thiourethane oligomers has been shown to increase fracture toughness and decrease polymerization stress in dental composites, though the mechanism is poorly understood. The aim of this study was to systematically characterize the effect of the type of filler surface functionalization on the physicochemical properties of experimental resin composites containing fillers of different size and volume fraction. Barium glass fillers (1, 3 and 10 µm) were functionalized with 2 wt% thiourethane-silane (TU-Sil) synthesized de novo and characterized by thermogravimetric analysis. Fillers treated with 3-(Trimethoxysilyl)propyl methacrylate (MA-Sil) and with no surface treatment (No-Sil) served as controls. Fillers (50, 60 and 70 wt%) were incorporated into BisGMA-UDMA-TEGDMA (5:3:2) containing camphorquinone/ethyl-4-dimethylaminobenzoate (0.2/0.8 wt%) and 0.2 wt% di-tert-butyl hydroxytoluene. The functionalized particles were characterized by thermogravimetric analysis and a representative group was tagged with methacrylated rhodamine B and analyzed by confocal laser scanning microscopy. Polymerization kinetics were assessed by near-IR spectroscopy. Polymerization stress was tested in a cantilever system, and fracture toughness was assessed with single edge-notched beams. Fracture surfaces were characterized by SEM. Data were analyzed with ANOVA/Tukey's test (α = 0.05). The grafting of thiourethane oligomer onto the surface of the filler particles led to reductions in polymerization stress ranging between 41 and 54%, without affecting the viscosity of the composite. Fracture toughness increased on average by 35% for composites with the experimental fillers compared with the traditional methacrylate-silanized groups. SEM and confocal analyses demonstrate that the coverage of the filler surface was not homogeneous and varied with the size of the filler. The average silane layer for the 1 µm particle functionalized with the thiourethane was 206 nm, much thicker than reported for traditional silanes. In summary, this study systematically characterized the silane layer and established structure–property relationships for methacrylate and thiourethane silane-containing materials. The results demonstrate that significant stress reductions and fracture toughness increases are obtained by judiciously tailoring the organic–inorganic interface in dental composites.https://doi.org/10.1038/s41598-021-87151-9
spellingShingle Ana Paula Piovezan Fugolin
Ana Rosa Costa
Lourenco Correr-Sobrinho
R. Crystal Chaw
Steven Lewis
Jack Liborio Ferracane
Carmem Silvia Pfeifer
Toughening and polymerization stress control in composites using thiourethane-treated fillers
Scientific Reports
title Toughening and polymerization stress control in composites using thiourethane-treated fillers
title_full Toughening and polymerization stress control in composites using thiourethane-treated fillers
title_fullStr Toughening and polymerization stress control in composites using thiourethane-treated fillers
title_full_unstemmed Toughening and polymerization stress control in composites using thiourethane-treated fillers
title_short Toughening and polymerization stress control in composites using thiourethane-treated fillers
title_sort toughening and polymerization stress control in composites using thiourethane treated fillers
url https://doi.org/10.1038/s41598-021-87151-9
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