GOALI: CDS&E: Computationally-Guided Development of Chromatographic Phases with Improved Retention Characteristics and of Sustainable Mobile Phases

在化学测量与成像计划的支持和界面工程计划的共同资助下，明尼苏达大学双子城分校的Siepmann教授和他的团队与Kround Gold Analytical的Mark Schure和高级材料技术公司的Stephanie Schuster一起研究用于分离化学混合物成分并进行分析的过程。具体地说，他们正在使用先进的模拟来获得对色谱分离过程的分子水平的理解。正如美国国家科学院最近在一份题为《转变分离科学的研究议程》的报告中强调的那样，分离科学在维持我们的生活水平和生活质量方面发挥着至关重要的作用。层析是一种重要的分离方法，它利用各种化学物质与填充在试管(色谱柱)中的颗粒相互作用的差异。当混合物通过色谱柱时，这些相互作用中的微小差异被放大，从而使一种化合物比另一种化合物更快地通过色谱柱，从而分离。这个大学-工业团队正在努力提高对颗粒表面的修改和对环境无害的溶剂的使用如何影响分离的理解，从而实现改进的化学分离系统。这一伙伴关系正在推进研究生、本科生和高中生的教育和培训，特别努力招收科学、技术、工程和数学等传统上代表性较低的群体的学生。这项工作与先进制造有关，因为分离是工业规模化学品生产中最昂贵和最耗时的方面之一。液体和超临界流体色谱的基本原理本质上是复杂的，由样品与固定相(多孔固体底物和键合配体)和流动相(通常是溶剂的混合物)的相互作用决定。Siepmann小组和Kround Gold Analytical正在使用蒙特卡罗和分子动力学模拟以及增强采样算法和可转移的分子力学力场来模拟和表征亲水固定相中的相互作用，包括两性离子相；通过添加亲水化合物调节灵活性和润湿性的新型疏水固定相；以及超临界二氧化碳和热压缩水流动相。该团队还利用粗粒模型来研究嵌段共聚物在表面多孔颗粒中的保留。先进材料技术公司正在领导一项进行协同色谱测量的努力。通过从这项工作中获得的分子水平的见解，改进了保留特性的固定相和可持续流动相的开发正在得到推进。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

With support from the Chemical Measurement & Imaging program, and co-funding from the Interfacial Engineering program, Professor Siepmann and his group at the University of Minnesota-Twin Cities together with collaborators Mark Schure at Kroungold Analytical and Stephanie Schuster at Advanced Materials Technology are investigating processes used to separate the components of chemical mixtures and enable their analysis. Specifically, they are using advanced simulations to obtain a molecular-level understanding of chromatographic separation processes. “Separation science plays a critical role in maintaining our standard of living and quality of life,” as recently emphasized by the National Academies in a report entitled "A Research Agenda for Transforming Separation Science." Chromatography is an important approach to separations that exploits differences in the interactions of various chemicals with particles packed into a tube (a chromatographic column). Small differences in these interactions get magnified as the mixture passes through the chromatographic column enabling one compound to move more quickly through the column than another and thus, separate. This university-industry team is working to improve understanding of how modifications of the particle surfaces and the use of environmentally benign solvents impact the separation, thereby enabling improved chemical separation systems. This partnership is advancing the education and training of graduate, undergraduate, and high school students, with special efforts made to recruit students from traditionally underrepresented groups in Science, Technology, Engineering and Mathematics. This effort has relevance to advanced manufacturing as separations is one of the most expensive and time-consuming aspects of the production of industrial scale chemicals.The underlying principles of liquid and supercritical fluid chromatography are inherently complex, being dictated by the interplay of the sample with the stationary phase (porous solid substrate and bonded ligands) and the mobile phase (often a mixture of solvents). The Siepmann group and Kroungold Analytical are using Monte Carlo and molecular dynamics simulations with enhanced-sampling algorithms and transferable molecular-mechanics force fields to model and characterize interactions in hydrophilic stationary phases including zwitterionic phases; novel hydrophobic stationary phases with limited flexibility and wettability tuned by the addition of hydrophilic compounds; and supercritical carbon dioxide and hot, compressed water mobile phases. The team is also utilizing coarse-grained models to investigate retention of block copolymers in superficially porous particles. Advanced Materials Technology is leading an effort to carry out synergistic chromatographic measurements. The development of both stationary phases with improved retention characteristics and sustainable mobile phases is being advanced through the molecular-level insights derived from this work.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.