Collaborative Research: Unraveling Interactions that Drive Water-Osmolyte Interactions in Confinement and Impact Self-Assembly

在这个由化学部门化学结构、动力学和机制A （CSDM-A）项目资助的合作项目中，Nancy Levinger教授（科罗拉多州立大学）和Bridget Gourley教授（德堡大学）和他们的研究小组正在使用磁和激光技术的结合来揭示水在纳米或大约400亿分之一英寸大小的微小结构中的动力学特性。在这些微小的环境中，水的分子行为与装满水的玻璃杯中的情况不同。此外，其他分子，如糖，通常在如此紧密的空间中与水一起发现，从根本上影响了水的性质。通过创建和表征一系列系统，这项工作促进了对水在环境中的行为的理解，这些行为对化学合成、环境修复、细胞活动等过程至关重要。参与该研究项目的学生在分子水平上发展专业知识，同时通过在不同职业阶段（本科、研究生和研究生）的跨机构科学家团队中一起工作，学习有效的项目协作技能。为了促进有效的指导，该项目还创建并评估了由pi领导的“导师导师”计划，以指导研究生研究人员成为更多新手研究人员的导师，从而培育下一代导师和科学家的发展。该程序采用一维和二维核磁共振以及时间分辨和稳态光学光谱来表征在反胶束中产生的受限环境以及其中发生的相互作用。结合这些工具的数据，揭示了约束和水渗透物相互作用的相互作用以及进料预测模型。描述了包裹渗透物的反胶束环境，结果揭示了这些环境如何影响质子和电子转移反应。此外，该项目还研究了水渗透物从体溶液到纳米环境的相互作用，并探讨了渗透物对反胶束结构、稳定性和形态的影响。该项目旨在通过开发预测工具，通过观察到的行为和提出的机制之间的直接相关性来揭示存在于受限水环境中的基本相互作用，从而提高知识水平。这个实验项目的广泛影响是双重的。首先，该项目为本科生和研究生提供核磁共振和时间分辨光谱学方面的重要培训，以及在多机构合作团队中工作的经验。这门科学揭示了渗透生物活跃的拥挤生物环境的细节，并提供了适用于食物、能源、水关系和生命规则等重大思想的预测模型。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

In this collaborative project funded by the Chemical Structure, Dynamics, and Mechanisms A (CSDM-A) Program of the Chemistry Division, Professors Nancy Levinger (Colorado State University) and Bridget Gourley (DePauw University) along with their research groups are using a combination of magnetic and laser techniques to shed light on water's dynamical properties when confined in minuscule structures that are nanometers, or approximately 40 billionths of an inch, in size. In these minuscule environments, water's molecular behavior does not match what happens in a glass full of water. Additionally, other molecules such as sugars, which are often found with water in such tight spaces, radically influence water’s properties. By creating and characterizing a range of systems, this work advances the understanding of water's behavior in environments that are important to processes such as chemical synthesis, environmental remediation, cellular activity, and beyond. Students involved in this research program develop expertise at the molecular level while with learning effective project collaboration skills by working together on an inter-institutional team of scientists at multiple career stages, undergraduate, graduate, and post-graduate. To facilitate effective mentoring the project also creates and assesses a "mentor the mentor" program led by the PIs to guide graduate researchers as mentors of more novice researchers and thus nurture the development of the next generation of mentors and scientists. This program employs 1D and 2D NMR along with time-resolved and steady-state optical spectroscopies to characterize the confined environments created in reverse micelles and the interactions occurring within them. Combining data from these tools reveals the interplay of confinement and water-osmolyte interactions and feed predictive models. Having characterized the reverse micelle environments that encapsulate osmolytes, results reveal how these environments affect proton and electron transfer reactions. Additionally, the project investigates water-osmolyte interactions transitioning from bulk solution to nanoscopic contexts and explores the impact of osmolytes on reverse micelle structure, stability, and form. The project seeks to advance knowledge by developing predictive tools through direct correlation between observed behaviors and proposed mechanisms to uncover fundamental interactions that exist in confined aqueous environments. The broader impacts of this experimental program are two-fold. First, the program provides undergraduate and graduate students important training in NMR and time-resolved optical spectroscopies as well as experience working in a multi-institutional collaborative team. The science reveals details about crowded biological environments where osmolytes are active and provide predictive models that apply to big ideas like the food, energy, water nexus, and Rules of Life.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.