Solid-State Nuclear Magnetic Resonance of Biomaterials

生物材料包括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的各种化学系统。由于无定形生物材料的无序性质，识别其分子水平结构本质上是困难的;历史上，研究人员一直依赖于试错法。核磁共振（NMR）光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核的能力促使NMR成为我们研究无序生物和无机材料的最强大的结构工具之一。我们的研究计划是使用固态核磁共振光谱来研究玻璃离子水门汀以及微晶玻璃和玻璃陶瓷。为了改善玻璃离子水门汀的生物功能和开发能够传递小分子的水门汀，需要详细了解网络修饰元素如何影响生物：无机界面的体积和表面结构。在这些复杂的化学系统中获得结构-性质关系的观点将最终导致我们设计从头材料的能力。 这项工作的目标是了解第三族元素如何影响目前在医学领域用于支持受损骨骼的磷硅酸盐玻璃内的生物活性反应。固态核磁共振还将用于研究玻璃离子水门汀作为无汞替代品用于牙科修复实践。由于这些生物材料中存在的某些改性阳离子很难检测，因此将研究磁场NMR的使用和高极化方法的发展。我们的目的是确定网络形成和修改阳离子的作用，在指导生物活性使用分层的方法进行研究和学生培训。作为物理化学家，我们提供必要的化学基础，以协助工程界弥合结构-性能差距，并在牙科和医学研究领域推进这些材料。因此，在加拿大的环境中，这项研究影响了整个生物材料界，同时提供了其他研究领域（例如，材料科学、工程学和地球科学）研究无序固体中局域和中程结构的开创性方法。

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.