Molecular level structure and dynamics of hydrated materials studied by NMR and IR spectroscopy

水合材料中水的结构和动力学性质对材料的功能起着关键作用。水合固体基质，如燃料电池中使用的聚合物，结缔组织中发现的生物大分子，以及阿尔伯塔省北部尾矿库中的水合粘土，都将其许多功能特性归因于水与材料的相互作用。开发在分子水平上研究水的新技术和方法是控制特定应用的水化材料性质的重要组成部分。在过去的六年中，我所在团队的本科生研究人员开发了各种多量子过滤技术，使我们能够使用2H核磁共振(核磁共振)光谱来测量剩余的四极耦合和自旋-自旋、T2、弛豫。这些参数有助于阐明水的局部结构以及分子如何在材料内从一个区域移动到另一个区域。我们建议的研究扩展了这些研究，结合了其他光谱技术来补充我们目前的方法。我们将利用红外光谱更好地了解氢键网络，利用场循环核磁共振弛豫法提供更完整的水动力学图景，并利用17O核磁共振光谱进一步揭示水的结构和动态性质。使用这套技术，我们将扩大我们对重要材料的水化特性的理解。具体地说，我们将研究通过在用于燃料电池的聚合物电解质膜中添加共聚物、增强层和无机成分而产生的新开发的杂化膜。这些添加剂旨在增加燃料电池的工作温度范围，并限制燃料种类的交叉(例如，甲醇燃料电池中的甲醇交叉)，从而提高燃料电池的性能。我们感兴趣的是这些修饰如何在一系列水化和温度范围内影响膜中的水行为。其次，我和学生们将继续我们的重要工作，将从脊柱组织获得的多个量子滤波的核磁共振信号与特定的生物标记物联系起来，为退行性腰椎间盘疾病的早期诊断提供基于磁共振的技术。我们在胶原蛋白方面的成功向我们展示了观察组织中单个大分子成分的价值，下一步将涉及聚集素和弹性蛋白的研究，以确定它们在组织中限制水运动的作用。最后，我们将利用我们研究水的能力来帮助当地工业更好地了解水与粘土的相互作用，并帮助开发技术，提供关于特定尾矿库样本的更详细的分子水平信息。

The structural and dynamic properties of water within hydrated materials play a key role in how materials function. Hydrated solid matrices such as the polymers used in fuel cells, biological macromolecules found in connective tissue, and hydrated clays in the tailings ponds of northern Alberta owe many of their functional properties to the interaction of water with the material. Developing new techniques and methodologies for studying water at the molecular level is an important part of controlling hydrated material properties for specific applications.In the past six years, undergraduate researchers in my group have developed various multiple quantum filtering techniques to allow us to measure the residual quadrupolar coupling and spin-spin, T2, relaxation, using 2H nuclear magnetic resonance (NMR) spectroscopy. These parameters help clarify the local structure of water and how the molecules move from region to region within the material. Our proposed research extends these studies, incorporating other spectroscopic techniques to complement our current methods. We will harness infrared spectroscopy to better understand hydrogen bond networks, field-cycling NMR relaxometry to provide a more complete picture of water dynamics, and 17O NMR spectroscopy to further unravel the structural and dynamic properties of water. Using this suite of techniques we will expand our understanding of the hydration properties of important materials. Specifically, we will study newly developed hybrid membranes created by adding copolymers, reinforcement layers, and inorganic components to polymer electrolyte membranes used in fuel cells. These additives are intended to increase the operating temperature range of the fuel cells and limit cross-over of fuel species, (e.g. methanol cross-over in methanol fuel cells) leading to higher fuel cell performance. We are interested in how these modifications affect water behavior in the membranes over a range of hydrations and temperatures. Secondly, the students and I will continue our important work of connecting the multiple quantum filtered NMR signal obtained from spinal disc tissue to specific biomarkers, providing magnetic resonance based techniques for early diagnosis of degenerative disc disease. Our success with collagen has shown us the value of looking at individual macromolecular components of the tissue and the next step will involve the study of aggrecan and elastin to determine their contributions to restricted water motion in tissue. Finally, we will use our ability to study water to assist local industries better understand water-clay interactions and help develop techniques that can provide more detailed molecular level information on specific tailings pond samples.