多功能多尺度齿科修复用无机材料可控制备机制和应用基础研究

Caries is regarded by WTO as one of three non-infectious diseases in 21st centuries. High performance organic-inorganic dental resin composites are a key for treatment. The related key science problems are how to realize high filling and excellent dispersion of inorganic fillers in dental resin composites. Nanosization, monodisperse and multiscale could resolve these problems. This project aims at the structure and function demands of dental inorganic fillers. Based on the control principle of molecular reaction engineering and functionally guided active design of surface, a novel “high gravity plus” route was presented, in which highly concentrated and stable monodisperse nanoparticles for dental resin composites are prepared by high gravity reaction crystallization-extraction separation technology, followed by “polymerization” technology based on spray-drying method for the building of microstructured nanoclusters. These nanoparticles or/and nanoclusters will be well dispersed in dental polymer matrix by high efficient process, thereby realizing low-cost preparation of high-performance dental resin composites. This project mainly investigates the preparation mechanism of monodisperse nanoparticles for dental resin composites by intensifying molecular mixing and mass transfer in a rotating packed bed reactor; explores the rules of mixing, mass transfer, particle nucleation, growth and dispersion in the coupling process of reaction, crystallization and extraction seperation; studies the interaction mechanism of nanoparticles and “polymerization” controlling rule in the atomization process; builds the structure-function relationship of preparation process, shape and structure, and application property.

龋病被世卫组织列为21世纪需重点防治的三大非传染性疾病之一，高品质有机无机复合树脂修复材料是治疗关键，涉及的关键问题是如何实现无机填料在其中的高填充和高分散，纳米化、单分散和多尺度可解决此问题。本项目针对齿科修复用无机填料结构和功能要求，基于分子反应工程调控原理和满足生物医用的表面修饰技术，提出采用“超重力+”法即超重力反应结晶-改性萃取技术宏量制备高浓度、高稳定齿科修复用单分散纳米颗粒液相分散体，并结合雾化成型“聚合”技术高效构筑多功能微米尺度纳米团簇体；进一步将单分散纳米颗粒和/或纳米团簇体高效复合分散于口腔树脂中，实现高性能齿科修复复合树脂材料的创制。重点研究齿科修复用单分散纳米颗粒可控制备的理论机制，探寻超重力环境下反应结晶-萃取分离过程中分子混合、传质、颗粒成核、生长与分散规律，探究雾化成型过程中纳米颗粒间作用机制和“聚合”调控规律，构建制备工艺-形态结构-应用性能间的本构关系。

龋病被世卫组织列为21世纪需重点防治的三大非传染性疾病之一，高品质有机无机复合树脂修复材料是治疗关键，涉及的关键问题是如何实现无机填料在其中的高填充和高分散，纳米化、单分散和多尺度可解决此问题。.本项目针对齿科修复用无机填料结构和功能要求，基于分子反应工程调控原理和满足生物医用的表面修饰技术，提出采用“超重力+”法即超重力反应结晶-改性萃取技术宏量制备高浓度、高稳定齿科修复用单分散纳米颗粒液相分散体，并结合雾化成型“聚合”技术高效构筑多功能微米尺度纳米团簇体；进一步将单分散纳米颗粒和/或纳米团簇体高效复合分散于口腔树脂中，实现高性能齿科修复复合树脂材料的创制。.本项目的研究内容和任务按计划已全面完成。本项目采用“超重力+”法，实现了SiO2、HAp、ZnO、ZrO2等纳米颗粒分散体的可控制备，揭示了合成机理和相关调控机制；与传统釜式法相比，“超重力+”法制备纳米分散体的反应时间明显缩短，所得产品颗粒粒径更小且分布更窄，分散性更好，可分散在不同极性介质中，最长可稳定分散12个月以上，分散体最高固含量可达60%，仍为透明。基于喷雾干燥的雾化成型“聚合”技术具有简便高效，所得产品形貌规整、分散性好等优点，所得纳微结构团簇体的填充性能明显优于一次纳米颗粒和相似尺寸的微米颗粒。本项目的成果将为多功能、多尺度高性能口腔无机纳微材料的主动设计、可控制备和应用提供了理论基础和技术支撑。本项目已在Chem. Eng. J.、Engineering、Ind. Eng. Chem. Res.、Dent. Mater.等国外权威期刊上发表论文14篇，其中SCI论文13篇；申请相关中国发明专利4件（已授权2件）；培养博士和硕士研究生7名。