高强纤维牙科复合树脂的界面增强增韧及其长效机制研究

After dental implants surgery, transitional fixed restoration is clinically significant to avoid oppression and absorption of alveolar bone as well as reconstruct soft tissue aesthetics. High-strength fiber composite resin is the first choice of transitional fixed restoration (crown and bridge) materials. This material is easy to operate, aesthetic, and has superior self-cleaning property. However, its oral service performance is poor during clinical use (half to one year) because the restoration is prone to break or fall off. All of these will eventually lead to the failure of transitional repair. Our project focused on the interface engineering research of quartz fiber prepared by high temperature process. We want to construct nanoscale precisely controlled amorphous nano-silica shell with high silicon hydroxyl density on the surface of quartz fiber through atomic layer deposition(ALD), and graft silane coupling agent uniformly. This will significantly improve the interface of inorganic and organic composite materials after light curing so as to improve its anti-drop property and long-term service performance. We will study the influence of sedimentation technique, coupling agent modification types, and technological conditions on the mechanical properties and service performance of composite resin, and optimize the technology to improve its performance. The dental high-strength fiber composite resin interface we explore in our project also has significant reference value on other dental restoration material properties, especially its long-term service performance.

牙种植术后过渡性固定修复体的使用对避免术区牙槽骨压迫吸收和重建软组织美学具有十分重要的临床意义。高强纤维复合树脂是种植术后制作过渡性修复体（冠、桥）的首选材料，具有易操作、美观、自洁功能好等特征，但其口内使用期间（0.5-1年）服役性能较差、修复体易折断和脱落，最终导致过渡性修复失败。本课题拟对高温工艺制备的石英纤维进行界面工程研究，通过原子层沉积（ALD）等技术在石英纤维表面构筑厚度纳米尺度精确可控、硅羟基密度高的非晶纳米二氧化硅壳层，均匀接枝硅烷偶联剂，显著改善光固化后无机有机复合材料的界面并籍此提高其防脱落和长期服役性能。研究沉积工艺、偶联剂改性种类及工艺条件等对复合物力学性能及服役性能的影响，不断优化工艺提高其性能。本项目探索的牙科高强纤维复合树脂界面工程途径，对其他口腔修复材料性能尤其长期服役性能同样有参考与借鉴价值。

高强纤维复合树脂材料是种植术后制作过渡性修复体（冠、桥）的首选材料，但其口内使用期间（0.5-1年）服役性能较差、修复体易折断和脱落，从而常导致过渡性修复失败。本课题对高温工艺制备的石英纤维进行界面工程研究，通过原子层沉积（ALD）等技术在石英纤维表面构筑厚度纳米尺度精确可控、硅羟基密度高的非晶纳米二氧化硅壳层，均匀接枝硅烷偶联剂，进行光固化后无机有机复合材料的界面研究。研究发现，ALD技术可以在石英纤维表面沉积超薄、共形、均一的纳米SiO2薄膜。通过表面结构表征发现经ALD处理后，纤维表面沉积了大量的硅元素与活性硅羟基，证明了SiO2薄膜的存在及其表面较强的化学活性；SEM观察发现沉积的纳米SiO2薄膜均匀、一致，进一步验证了薄膜的超薄性与共形性。在此基础上，通过调节ALD不同参数，发现薄膜随着循环周期的增加，其沉积厚度呈线性增长关系，每沉积一个周期，薄膜厚度增加0.046nm。ALD技术沉积的SiO2薄膜与石英纤维表面发生强有力的化学结合，使得制备的纤维树脂复合物力学强度显著提高（与前期研究中表面接枝处理方法相比提高53%，与未使用ALD技术相比提高28%），有效弥补了临床上高强纤维复合树脂过渡性修复体强度不足、易折断和脱落的缺陷，从而进一步提高其口内服役性能。在已取得的研究结果基础上，本课题将ALD技术扩展应用于提高牙科ZrO2陶瓷表面粘结性能的研究中，发现在惰性ZrO2表面通过ALD技术可以沉积相同特点的纳米SiO2薄膜。该薄膜使得ZrO2/树脂短期、长期粘接强度分别提高27%与24%（与临床常用ZrO2表面处理剂MDP方法相比）。本项目探索的牙科高强纤维树脂复合物界面工程途径，对其他口腔修复材料性能尤其长期服役性能同样有参考与借鉴价值。