CDS&E: Theoretical, Numerical and Experimental Analysis of Gas-Ion Energy Exchange in Ion Mobility for the Separation of Polyatomic Ions

CDS

• 批准号: 2203968
• 负责人: Carlos Larriba Andaluz
• 金额: $ 39.22万
• 依托单位: Indiana University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-09-01 至 2026-08-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2203968&HistoricalAwards=false
• 关键词: CDS& Theoretical; Numerical; Experimental; Analysis

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Carlos Larriba-Andaluz and his group at Indiana University-Purdue University in Indianapolis are working on improving the understanding of how ionic compounds may be separated and characterized in the gas phase via a technique known as Ion Mobility Spectrometry (IMS). Understanding how this separation occurs is not only vital to analytical chemistry, but also to aerosol science and plasma physics. One of the reasons that IMS has become quite relevant is that it is able to distinguish ions that have the same mass but different shapes, known as isomers. Distinguishing isomers is extremely important - small changes in shape can result in drastic changes in chemical and physical properties. In fact, IMS systems have arrived at such sophistication that the existing theory is incapable of describing some of the observed separation capabilities. The Larriba-Andaluz group is working to fill this knowledge gap through novel theoretical approaches and numerical tools. The team is engaging undergraduate students, including members of underrepresented groups, through summer courses. They are also developing online IMS training materials to captivate both new and seasoned users.Ion Mobility Spectrometry (IMS) is becoming one of techniques most employed in combination with Mass Spectrometry (MS). As IMS systems become more sensitive and accurate, commonly used modeling and theory approximations have been unable to explain some recently observed capabilities, including separations of isomers, isotopologues, and even isotopomers. Interchange of energy between translational and internal degrees of freedom accompanying ion-molecule collisions is a potential contributor to these phenomena which has not yet been incorporated into existing theories. The Larriba-Andaluz group is investigating the mechanism and role of this energy exchange under conditions of varying electric field and temperature. Specifically, they are developing 1) higher-order ion mobility approximations using two-temperature theory, followed by the inclusion of ion energy calculations and inelasticity effects, and 2) models of mobility and energy balance using an in-house Molecular Dynamics-Monte Carlo hybrid code. Comparison of experimental results at different fields and temperatures is being used to predict the effect of inelastic contributions. The resulting insights are expected to help explain the remarkable separation ability of ion mobility spectrometry and to broadly advance the field of ion mobility.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.

在化学划分的化学测量和成像计划的支持下，印第安纳波利斯印第安纳大学普尔德大学的Carlos Larriba-Andaluz及其小组正在努力通过一种通过一种已知的AS ICOM迁移率（IMS）在气相中分离和表征对离子化合物的理解。了解这种分离的发生方式不仅对分析化学，而且对气溶胶科学和血浆物理学至关重要。 IMS变得非常相关的原因之一是，它能够区分具有相同质量但形状不同的离子（称为异构体）的离子。区分异构体非常重要 - 形状的小变化会导致化学和物理性质的急剧变化。实际上，IMS系统已经达到了如此复杂，以至于现有理论无法描述某些观察到的分离能力。 Larriba-Andaluz小组正在努力通过新颖的理论方法和数值工具来填补这一知识差距。该团队通过夏季课程与本科生，包括代表性不足的团体成员。 他们还在开发在线IMS培训材料，以吸引新的和经验丰富的用户。ION移动光谱法（IMS）正在成为与质谱法（MS）结合使用的技术之一。随着IMS系统变得更加敏感和准确，常用的建模，理论近似无法解释一些最近观察到的功能，包括异构体，同位素学甚至同位素的分离。 伴随离子 - 分子碰撞的自由度和内部自由度之间的能量互换是这些现象的潜在贡献者，这些现象尚未纳入现有理论。 Larriba-Andaluz组正在研究这种能量交换的机制和作用，在不同的电场和温度条件下。具体而言，它们正在开发1）使用两个温度理论的高阶离子迁移率近似，然后使用离子能量计算和非弹性效应，以及2）使用内部分子动力学 - 蒙特卡洛杂种杂交代码的迁移率和能量平衡的模型。 在不同场和温度下实验结果的比较正在用于预测非弹性贡献的影响。预计所产生的见解将有助于解释离子移动光谱法的显着分离能力，并广泛推进离子移动性领域。该奖项反映了NSF的法定任务，并被认为值得通过基金会的智力优点和更广泛的影响来通过评估来获得支持。

项目成果

A critical review of the two-temperature theory and the derivation of matrix elements. High field ion mobility and energy calculation for all-atom structures in light gases using a 12-6-4 potential

对双温度理论和矩阵元素推导的批判性回顾。

• DOI: 10.1016/j.talo.2023.100191
• 发表时间: 2023
• 期刊: Talanta Open
• 作者: Gandhi, Viraj D.;Hua, Leyan;Chen, Xuemeng;Latif, Mohsen;Larriba-Andaluz, Carlos
• 通讯作者: Larriba-Andaluz, Carlos

A numerical tool to calculate ion mobility at arbitrary fields from all-atom models

从全原子模型计算任意场的离子淌度的数值工具

• DOI: 10.1016/j.jaerosci.2022.106122
• 发表时间: 2023
• 期刊: Journal of Aerosol Science
• 影响因子: 4.5
• 作者: Gandhi, Viraj D.;Short, Kyle;Hua, Leyan;Rodríguez, Iván;Larriba-Andaluz, Carlos
• 通讯作者: Larriba-Andaluz, Carlos