Dental Composite Materials Based on Photoinitiated Thiol-Vinyl Sulfone Reactions

基于光引发硫醇-乙烯基砜反应的牙科复合材料

• 批准号: 8610759
• 负责人: Christopher N Bowman
• 金额: $ 45.83万
• 依托单位: UNIVERSITY OF COLORADO
• 依托单位国家: 美国
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-09-01 至 2018-08-31
• 项目状态: 已结题
• 来源: https://reporter.nih.gov/project-details/8610759
• 关键词: Adhesives; Appearance; Behavior; Biocompatible; Biocompatible Materials; Biological; Chemical Structure; Clinical; Communities; Complex; Conflict (Psychology); Coupling; Dental; Dental Esthetics; Dental General Practice; Dental Materials; Dental caries; Development; Environment; Esters; Excision; Extravasation; Failure; Fatigue; Filler; Goals; Grant; In Situ; Lead; Left; Life; Mechanical Stress; Mechanics; Methacrylates; Modification; Oral; Performance; Phase; Plague; Plant Resins; Polymers; Process; Property; Reaction; Rupture; Scheme; Series; Services; Solutions; Stress; Structure; Sulfhydryl Compounds; Swelling; System; Testing; Tooth structure; absorption; base; biomaterial compatibility; chemical reaction; composite restoration; dental resin; divinyl sulfone; functional group; improved; mechanical behavior; monomer; novel; novel strategies; oral biofilm; polymerization; premature; prevent; public health relevance; restoration; restorative composite; restorative dentistry; restorative material; triethylene glycol dimethacrylate

DESCRIPTION (provided by applicant): Dental restorations represent one of the conceptually simplest biomaterials - essentially requiring the restoration of mechanical function in an aesthetically acceptable manner. Yet, despite that conceptual simplicity, an array of complex and often conflicting material, biological, curing and reaction properties necessitate a series of suboptimal solutions. Hundreds of millions of restorations are performed each year and premature failure of these restorations results in the need for a far greater number of restorations, including the occasional removal of additional healthy tooth structure. The need for simple, biocompatible, easily manipulated aesthetic dental restoratives has pushed the community towards polymeric composites that are readily reacted in situ, generally by photoinitiation, to yield a high modulus, high strength composite structure that is tooth-like in appearance. Despite the importance of these materials, the resin (i.e., the polymerizable component) phase of these systems has remained largely unchanged since its introduction several decades ago. The common use of dimethacrylate-based resins for dental restorative materials is plagued by critical problems; they do not achieve complete conversion of the methacrylates and thus leave a great deal of material that can be extracted into the oral environment. Further, these materials are prone to significant shrinkage and shrinkage stress that arises during the polymerization/curing process that is used to set the material. Thus, here, we propose a revolutionary new approach to dental materials based on the nucleophile- catalyzed thiol-vinyl sulfone network forming reaction. The proposed thiol-vinyl sulfone dental composite system will significantly improve upon the biological, chemical reaction and mechanical behavior of traditional methcrylate based composite systems. Based on exciting preliminary results that demonstrate the ability to achieve complete functional group conversion via this highly efficient, rapid reaction; appropriate mechanical behavior from the polymers formed; low shrinkage and stress; and the elimination of enzymatically reactive functional groups from the resin, we hypothesize that resins formed by this thiol-vinyl sulfone reaction represent ideal candidates as dental restorative materials. The overall aim is to develop and evaluate dental composites based on the nucleophile catalyzed thiol-vinyl sulfone Michael addition reaction that will include the development of appropriate monomers and functionalized fillers, the development of highly reactive photoinitiator systems for these resins, and the demonstration of acceptable fatigue, extractables, biocompatibility, degradation and other essential short- and long-term composite behavior. Ultimately, the overall aim is to establish these thiol-vinyl sulfone-based composites as a disruptive change in the dental composite field. We will demonstrate over the course of this grant period that these materials are capable of achieving more than a two-fold increase in service lifetime based on dramatically reduced extractables, swelling, degradation and wear in longterm, environmentally challenging testing conditions.

描述（由申请人提供）：牙科修复体代表了概念上最简单的生物材料之一-本质上要求以美学可接受的方式恢复机械功能。然而，尽管概念简单，但一系列复杂且经常相互冲突的材料，生物，固化和反应特性需要一系列次优解决方案。每年进行数以亿计的修复，这些修复的过早失败导致需要更多的修复，包括偶尔去除额外的健康牙齿结构。对简单的、生物相容性的、易于操作的美观牙科修复体的需求推动了聚合物复合材料的发展，这种材料通常通过光引发，易于在原位反应，从而产生高模量、高强度的复合材料结构，其外观与牙齿相似。尽管这些材料很重要，但自几十年前引入以来，这些系统的树脂（即可聚合组分）相基本保持不变。二甲基丙烯酸酯基树脂在牙科修复材料中的普遍应用存在一些关键问题；它们不能实现甲基丙烯酸酯的完全转化，因此留下了大量可以被提取到口腔环境中的物质。此外，这些材料在用于固化材料的聚合/固化过程中容易产生显著的收缩和收缩应力。因此，在这里，我们提出了一种基于亲核试剂催化的巯基乙烯砜网络形成反应的牙科材料的革命性新方法。所提出的巯基-乙烯砜牙科复合体系将显著改善传统的甲基丙烯酸酯基复合体系的生物、化学反应和力学性能。基于令人兴奋的初步结果，表明能够通过这种高效，快速的反应实现完整的官能团转换；形成的聚合物具有适当的机械性能；低收缩率和应力；并且从树脂中去除酶活性官能团，我们假设由这种巯基乙烯砜反应形成的树脂代表了牙科修复材料的理想候选者。总体目标是开发和评估基于亲核试剂催化的巯基-乙烯基砜迈克尔加成反应的牙科复合材料，包括开发合适的单体和功能化填料，开发用于这些树脂的高活性光引发剂系统，以及展示可接受的疲劳，可提取性，生物相容性，降解和其他必要的短期和长期复合行为。最终，总体目标是建立这些基于巯基乙烯砜的复合材料作为牙科复合材料领域的颠覆性变革。在此资助期间，我们将证明这些材料能够在长期、具有环境挑战性的测试条件下显著减少可提取、膨胀、降解和磨损，从而将使用寿命延长两倍以上。