Solid-State Nuclear Magnetic Resonance of Biomaterials

生物材料包括各种化学体系，从生物活性催化剂到具有化学调节特定功能的巨大潜力的无定形结构支架。由于非晶态生物材料的无序性质，识别其分子级结构本身就很困难；从历史上看，研究人员一直依赖于一种反复试验的方法。核磁共振波谱是一种对局部化学环境敏感的非破坏性技术。这种独特的局部探测和调谐特定原子核的能力促使核磁共振成为我们可以使用的最强大的结构工具之一，用于研究无序的生物和无机材料。我们提出的研究是利用固体核磁共振波谱来研究玻璃离子水门汀以及生物玻璃和微晶玻璃。为了改善玻璃离子水门汀的生物功能，开发能够输送小分子的生物玻璃，需要详细了解网络修饰元件如何影响生物-无机界面的整体和表面结构。了解这些复杂化学体系中的结构-性质关系将最终导致我们有能力设计从头开始的材料。 这项工作的目标是了解第三族元素如何影响目前医学领域中用于支持受损骨骼的磷硅酸盐生物玻璃的生物活性反应。固态核磁共振还将用于研究玻璃离子粘固剂作为修复牙科实践中的无汞替代品。由于这些生物材料中存在的某些修饰阳离子很难检测到，因此超高场核磁共振的使用和高极化方法的发展将被研究。我们的目的是确定网络形成和修饰阳离子在使用分级方法进行研究和学生培训时在指导生物活性方面所起的作用。作为物理化学家，我们提供必要的化学基础，以帮助工程界弥合结构-性能差距，并在牙科和医学研究领域推动这些材料的发展。因此，在加拿大环境中，这项研究影响了整个生物材料社区，同时提供了其他研究领域(如材料科学、工程学和地球科学)的开创性方法，以研究无序固体中的局部和中期结构。

Biomaterials encompass a diverse range of chemical systems from bioactive catalysts to amorphous structural scaffolds with tremendous potential for chemically tuning specific functions. Identifying molecular-level structure of amorphous biomaterials is inherently difficult due to their disordered nature; historically, researchers have relied on a trial-and-error approach. Nuclear magnetic resonance (NMR) spectroscopy is a non-destructive technique that is sensitive to the local chemical environment. This unique ability to probe locally and tune to specific nuclei has prompted NMR to become one of the most powerful structural tools at our disposal to study disordered biological and inorganic materials. Our proposed research is to use solid-state NMR spectroscopy to study glass ionomer cements as well as bioglasses and glass-ceramics. To improve biological function of glass ionomer cements and develop bioglasses capable of small molecule delivery requires a detailed understanding of how network-modifying elements affect bulk and surface structure at the biological:inorganic interface. Gaining a perspective on the structure-property relationships within these complex chemical systems will ultimate lead to our ability to design de novo materials. The target of this work is to understand how group III elements affect bioactive responses within phosphosilicate bioglasses currently used within the medical field to support damaged bones. Solid-state NMR will also be used to study glass ionomer cements used as mercury-free alternatives for restorative dental practices. As certain modifying cations present in these biomaterials are difficult to detect, the use of ultrahigh field NMR and the development of high-polarization approaches will be studied. Our intent is to identify the roles network-forming and modifying cations have in directing bioactivity using a tiered approach to research and student training. As physical chemists we provide the chemical foundations essential to assist the engineering community in bridging the structure-property gap and advance these materials in the dental and medical research fields. As such within the Canadian environment this research impacts the biomaterials community at large while providing other research fields (e.g., materials science, engineering, and earth science) pioneering methods to investigate local- and medium-range structure within disordered solids.