Deciphering and quantifying molecular interactions driving self-assembly and fibrillar growth in organogels

罗杰斯博士的研究计划的目的是开发一种基本的，自下而上的分子凝胶自组装方法，希望回答这个问题：为什么一些简单的小分子自组装成纳米组装体，包括纤维，带状物和胶囊？将研究在各种溶剂中的胆甾醇衍生分子的结构与其纳米结构、微观结构和超分子结构之间的关系。目的是1）什么官能团增强D-山梨醇衍生分子的自组装; 2）分子间力如何驱动组装成不同的超分子结构（例如，纤维对带）;以及3）分子结构和非共价相互作用的变化如何改变与凝胶形成相关的汉森空间区域。具体来说，罗杰斯博士将专注于分子凝胶，来自糖（即，山梨醇），长期目标是通过将食用油纳米结构化为固体来减少加工食品中的反式脂肪。通过对这些数据的系统评价，将解决以下问题：（1）在自组装纤维网络（SAFiN）中，哪些官能团增强了自组装？和（2）分子间力如何驱动组装成不同的超分子结构（例如，纤维、带状物等）。这些相关性将成为开发工具的基础，使科学界能够采用合理的设计来开发新的胶凝剂。这将是迄今为止关于溶剂和胶凝剂分子特性对自组装成分子凝胶的作用的最全面和完整的研究！预测参数将被开发，以确定为什么一些小分子自组装成纤维在特定的溶剂和其他不，信息，可以解释聚集过程的起源在自然界中。拟议的研究是高度跨学科的，PI将利用多学科培训的学生。先验的工具，建立在这个NSERC DG，将使新的小分子能够形成分子凝胶，不仅可以结构食用油，但也有应用于光化学，光收集，控制药物释放，和成核聚合物，所有这些目前正在研究中的发现。

The aim of Dr. Rogers’ research program is to develop a fundamental, bottom-up approach to self-assembly in molecular gels, in hopes of answering the question: why do some simple small molecules self-assemble into nano-assemblies, including fibers, ribbons and capsules? The relationships between the structures of sorbitol-derived molecules and their nanostructural, microstructural, and supramolecular architectures in various solvents will be investigated. The objectives are 1) what functional groups enhance self-assembly of the D-sorbitol derived molecules; 2) how intermolecular forces drive assembly into different supramolecular structures (e.g., fibers versus ribbons); and 3) how changes in molecular structure and non-covalent interactions alter the regions of Hansen space that correlates to the formation of gels. Specifically, Dr. Rogers will focus on molecular gels, derived from sugars (i.e., sorbitol), with the long-term goal to reduced trans fats in processed foods by nanostructuring edible oils into solids. By systematically evaluating the data, the following queries will be addressed: (1) What functional groups enhance self-assembly in self-assembled fibrillar networks (SAFiNs)?; and (2) How do intermolecular forces drive assembly into different supramolecular structures (e.g., fibers, ribbons, etc.)? These correlations will be a basis for developing tools allowing the scientific community to employ rational designs to develop new gelators. This will be the most comprehensive and complete study to date on the roles of solvent and gelator molecular characteristics on self-assembly into molecular gels! Predictive parameters will be developed to determine why some small molecules self-assemble into fibers in specific solvents and other do not, information that may explain the origins of aggregation processes in nature. The proposed research is highly interdisciplinary and the PI will utilize multidisciplinary training for the students. The a priori tools, established in this NSERC DG, will enable the discovery of new small molecules capable of forming molecular gels that can not only structure edible oils but also have applications in photovoltaics, light harvesting, controlled drug release, and nucleating polymers, all of which are currently being investigated.