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

目标：CDS

• 批准号: 2003246
• 负责人: Joern Ilja Siepmann
• 金额: $ 44.96万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2003246&HistoricalAwards=false
• 关键词: GOALI; CDS& Computationally; Guided; Development

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.

在化学测量与成像项目的支持下，以及界面工程项目的共同资助下，明尼苏达大学双城分校的 Siepmann 教授及其团队与 Kroungold Analytical 的 Mark Schure 和先进材料技术公司的 Stephanie Schuster 合作者正在进行研究具体来说，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了解。正如美国国家科学院最近在题为“变革分离科学的研究议程”的报告中所强调的那样，色谱法是一种重要的分离方法，它利用了各种化学物质与填充颗粒之间相互作用的差异。当混合物通过色谱柱时，这些相互作用的微小差异会被放大，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。团队正在努力提高对颗粒表面的修饰和环境友好溶剂的使用如何影响分离的理解，从而改进化学分离系统，这种合作关系正在推进研究生、本科生和高中生的教育和培训。特别努力从传统上代表性不足的科学、技术、工程和数学群体中招收学生。这项努力与制造先进的分离有关，这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本质上是复杂的，由样品与固定相（多孔固体基质和键合配体）和流动相（通常是溶剂的混合物）的相互作用决定。Siepmann 小组和 Kroungold Analytical 使用蒙特卡罗和分子动力学。使用增强采样算法和可转移分子力学力场进行模拟，以模拟和表征亲水固定相（包括具有有限灵活性的新型疏水固定相）的相互作用；通过添加亲水性化合物来调节润湿性；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。两种固定相的开发反映了保留特性的改进，而可持续流动相正在通过这项工作获得的分子水平见解得到推进。该奖项是 NSF 的法定使命，被认为是值得的。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来获得支持。

项目成果

Characterization of Functionalized Chromatographic Nanoporous Silica Materials by Coupling Water Adsorption and Intrusion with Nuclear Magnetic Resonance Relaxometry

• DOI: 10.1021/acsanm.3c04330
• 发表时间: 2024-01
• 期刊: ACS Applied Nano Materials
• 影响因子: 5.9
• 作者: Carola Schlumberger;Carlos Cuadrado Collados;Jakob Söllner;Christoph Huber;D. Wisser;Hsiao-Feng Liu