Acta Biomaterialia ( IF 9.4 ) Pub Date : 2017-12-08 , DOI: 10.1016/j.actbio.2017.12.001 Linyong Song 1 , Qiang Ye 1 , Xueping Ge 1 , Anil Misra 2 , Candan Tamerler 3 , Paulette Spencer 3
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Ingress of bacteria and fluids at the interfacial gaps between the restorative composite biomaterial and the tooth structure contribute to recurrent decay and failure of the composite restoration. The inability of the material to increase the pH at the composite/tooth interface facilitates the outgrowth of bacteria. Neutralizing the microenvironment at the tooth/composite interface offers promise for reducing the damage provoked by cariogenic and aciduric bacteria. We address this problem by designing a dental adhesive composed of hybrid network to provide buffering and autonomous strengthening simultaneously. Two amino functional silanes, 2-hydroxy-3-morpholinopropyl (3-(triethoxysilyl)propyl) carbamate and 2-hydroxy-3-morpholinopropyl (3-(trimethoxysilyl)propyl) carbamate were synthesized and used as co-monomers. Combining free radical initiated polymerization (polymethacrylate-based network) and photoacid-induced sol-gel reaction (polysiloxane) results in the hybrid network formation. Resulting formulations were characterized with regard to real-time photo-polymerization, water sorption, leached species, neutralization, and mechanical properties. Results from real-time FTIR spectroscopic studies indicated that ethoxy was less reactive than methoxy substituent. The neutralization results demonstrated that the methoxy-containing adhesives have acute and delayed buffering capabilities. The mechanical properties of synthetic copolymers tested in dry conditions were improved via condensation reaction of the hydrolyzed organosilanes. The leaching from methoxy containing copolymers was significantly reduced. The sol-gel reaction provided a chronic and persistent reaction in wet condition-performance that offers potential for reducing secondary decay and increasing the functional lifetime of dental adhesives.
Statement of Significance
The interfacial gaps between the restorative composite biomaterial and the tooth structure contributes to recurrent decay and failure of the composite restoration. The inability of the material to increase the pH at the composite/tooth interface facilitates the outgrowth of more cariogenic and aciduric bacteria.
This paper reports a novel, synthetic resin that provides buffering capability and autonomous strengthening characteristics. In this work, two amino functional silanes were synthesized and the effect of alkoxy substitutions on the photoacid-induced sol-gel reaction was investigated. We evaluated the neutralization capability (monitoring the pH of lactic acid solution) and the autonomous strengthening property (monitoring the mechanical properties of the hybrid copolymers under wet conditions and quantitatively analyzing the leachable species by HPLC). The novel resin investigated in this study offers the potential benefits of reducing the risk of recurrent decay and prolonging the functional lifetime of dental adhesives.
中文翻译：
具有牙科粘合剂缓冲能力和自主增强特性的混合交联网络的制造。
细菌和液体进入修复复合生物材料和牙齿结构之间的界面间隙会导致复合修复体反复腐烂和失效。该材料无法提高复合材料/牙齿界面的 pH 值，从而促进了细菌的生长。中和牙齿/复合材料界面处的微环境有望减少致龋菌和酸尿菌引起的损害。我们通过设计一种由混合网络组成的牙科粘合剂来解决这个问题，以同时提供缓冲和自主强化。合成了两种氨基官能硅烷，2-羟基-3-吗啉代丙基(3-(三乙氧基甲硅烷基)丙基)氨基甲酸酯和2-羟基-3-吗啉代丙基(3-(三甲氧基甲硅烷基)丙基)氨基甲酸酯并用作共聚单体。将自由基引发聚合（基于聚甲基丙烯酸酯的网络）和光酸诱导的溶胶-凝胶反应（聚硅氧烷）相结合，形成杂化网络。所得配方的特征包括实时光聚合、吸水性、浸出物质、中和和机械性能。实时 FTIR 光谱研究的结果表明，乙氧基取代基的反应性低于甲氧基取代基。中和结果表明含甲氧基粘合剂具有急性和延迟缓冲能力。在干燥条件下测试的合成共聚物的机械性能通过水解有机硅烷的缩合反应得到改善。含甲氧基共聚物的浸出显着减少。溶胶-凝胶反应在潮湿条件下提供了慢性且持久的性能反应，为减少二次腐烂和延长牙科粘合剂的使用寿命提供了潜力。
重要性声明
修复复合生物材料和牙齿结构之间的界面间隙导致复合修复体反复腐烂和失效。该材料无法提高复合材料/牙齿界面的 pH 值，从而促进了更多致龋菌和耐酸菌的生长。
本文报道了一种新型合成树脂，具有缓冲能力和自主强化特性。在这项工作中，合成了两种氨基官能硅烷，并研究了烷氧基取代对光酸诱导的溶胶-凝胶反应的影响。我们评估了中和能力（监测乳酸溶液的 pH 值）和自主增强性能（监测湿条件下杂化共聚物的机械性能并通过 HPLC 定量分析可浸出物质）。本研究中研究的新型树脂具有降低反复腐烂风险和延长牙科粘合剂使用寿命的潜在好处。
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