Nuclear Magnetic Resonance Studies of Molecular Structure and Dynamics

分子结构和动力学的核磁共振研究

• 批准号: RGPIN-2019-06816
• 负责人: Wasylishen, Roderick
• 金额: $ 2.62万
• 依托单位: University of Alberta
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2020
• 资助国家: 加拿大
• 起止时间: 2020-01-01 至 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=716227
• 关键词: Nuclear; Magnetic; Resonance; Studies; Molecular

The research proposal describes a program to investigate the detailed structure and dynamics of materials that are of fundamental interest to the scientific community. A wide range of materials will be investigated including hybrid perovskites that are building blocks of solar cells, natural products and pharmaceuticals that are important in medicine, and transition metal complexes, some of which catalyze chemical reactions and have important industrial applications. Our principal experimental tool for investigating the structure and dynamics of materials is nuclear magnetic resonance spectroscopy, a general tool upon which MRI, magnetic resonance imaging, is based. Many of the natural products that we examine, e.g., curcumin, have strong hydrogen bonds that play a fundamental role in determining their molecular structure and hence their molecular properties. In these molecules with intramolecular hydrogen bonds we have very recently observed deuterium isotope effects on NMR chemical shifts in the solid state that we believe have the potential to provide detailed information about the positions of hydrogen atoms, information difficult to obtain by X-ray diffraction. We are working with theoreticians to compute accurate potentials and zero-point energies for systems with unsymmetrical double-well potential surfaces. It is interesting to point out that the US FDA has approved the first deuterium-labeled drug, tetrabenazine-d6, for human use. We have extensive experience working with methylammonium lead iodide, a compound that belongs to a class of compounds known as organic-inorganic hybrid perovskites. Although we started working with this material in 1985, not long after it was first prepared by Weber, it was not until 2009 that it was realized that this material could be used to convert solar energy into electrical energy. In 2009, the efficiency of converting solar energy to electrical energy was approximately 3.8 %, but now, by careful control of the preparation procedures, efficiencies in excess of 22% have been achieved. Today, we join many research groups scrutinizing related organic-inorganic perovskite materials as possible candidates for solar energy applications. From the recent literature, it seems clear that the cation and halide ion dynamics significantly influences the performance of these materials. We plan to use mechanochemical synthetic methods to prepare several lead mixed-halide perovskites and characterize both the cation and anion dynamics using solid-state NMR.

研究建议描述了一项计划，以调查科学界基本兴趣的材料的详细结构和动态。 将研究广泛的材料，包括混合钙壶，它们是在医学中很重要的太阳能电池，天然产物和药物的基础，以及过渡金属复合物，其中一些催化了化学反应并具有重要的工业应用。 我们研究材料结构和动力学的主要实验工具是核磁共振光谱，这是一种通用工具，MRI（磁共振成像）基于该工具。 我们检查的许多天然产物，例如姜黄素，具有强大的氢键，它们在确定其分子结构并因此具有分子特性方面起着基本作用。 在这些具有分子内氢键的分子中，我们最近观察到同位素对固态NMR化学移位的影响，我们认为我们认为有可能提供有关氢原子位置的详细信息，这是X射线衍射难以获得的信息。我们正在与理论家合作，以计算具有不对称双孔电势表面的系统的准确势和零点能量。 有趣的是指出，美国FDA批准了第一种用于人类使用的氘标记的药物Tetrabenazine-D6。 我们有丰富的经验与甲基二铅碘化物合作，该化合物属于一类称为有机无机杂化钙钛矿的化合物。 尽管我们从1985年开始使用这种材料，但在韦伯首次制备之后不久，直到2009年才意识到该材料可用于将太阳能转化为电能。 在2009年，将太阳能转换为电能的效率约为3.8％，但现在，通过仔细控制制备程序，已经达到了超过22％的效率。 今天，我们加入了许多研究小组，审查相关的有机无机钙钛矿材料作为太阳能应用的可能候选者。 从最近的文献来看，阳离子和卤化离子动力学似乎显着影响这些材料的性能。 我们计划使用机械化学合成方法来制备几种混合卤化物钙钛矿，并使用固态NMR表征阳离子和阴离子动力学。