Advancing QM/MM Methods to Model Reactions in Ionic Fluids

有了这个奖项，化学部的化学理论，模型和计算方法（CTMC）计划资助奥本大学的奥兰多阿切韦多和杰弗里奥弗比开发和应用离子液体的理论和计算方法。 高级网络基础设施部门的计算和数据支持科学与工程（CDS E）计划为该奖项做出了贡献。每年处理的化学废物超过1亿磅，更好地了解如何优化化学反应的可回收溶剂有可能影响从实验室工作台到大规模工业制造的社会。离子液体是一种完全由离子组成的可回收溶剂，具有加速和控制广泛反应的能力。然而，最近出现了一种称为深共晶溶剂（DES）的新的离子流体家族，作为环境更安全且相对便宜的替代品。作为化学反应的介质，每种溶剂类别都有明显的优势;然而，DES才刚刚开始成为潜在的替代品。目前的研究将有助于建立一个坚实的理解分子间的相互作用发生在整个化学反应时，溶剂化的离子液体和DES。该策略是采用高端计算建模来阐明这些离子流体对重要化学反应产物形成机制的影响。将为化学科学和软件开发的学生提供交叉培训，为STEM劳动力做好准备。该提案还将通过一个动手的即时超级计算机研讨会向高中和本科生介绍计算化学，该研讨会以建造一台临时超级计算机为特色。奥兰，奥弗比和工人们研究了离子流体引起的化学反应性增强，并开发了QM/MM方法的新进展。我们的目标是使用QM/MM模拟解决争议的影响，离子液体和DES速率加速，机制，和%ee增强相比，传统的溶剂。提出了多种氯化胆碱类DES溶剂和1-烷基-3-甲基咪唑类离子液体的力场参数的发展。此外，将向科学模拟界免费提供一个高度并行的开放源码软件包，用于执行QM/MM计算。

With this award, the Chemical Theory, Models and Computational Methods (CTMC) Program in the Chemistry Division is funding Orlando Acevedo and Jeffrey Overbey of Auburn University to develop and apply theoretical and computational approaches for ionic liquids. The Computational and Data-Enabled Science and Engineering (CDS&E) program in the Division of Advanced Cyberinfrastructure is contributing to the award. With over 100 million pounds of chemical waste treated yearly, a better understanding of how to optimize recyclable solvents for chemical reactions has the potential to impact society from the lab bench top to large-scale industrial manufacturing. Ionic liquids, recyclable solvents composed exclusively of ions, have the ability to accelerate and control a vast range of reactions. However, a new family of ionic fluids called deep eutectic solvents (DES) has recently emerged as an environmentally safer and relatively inexpensive alternative. As a medium for chemical reactions each solvent class has distinct advantages; however, the DES are only beginning to emerge as a potential substitute. The current study will help establish a firm understanding of the intermolecular interactions occurring throughout chemical reactions when solvated by ionic liquids and DES. The strategy is to employ high-end computational modeling to elucidate the effect of these ionic fluids upon the mechanism of product formation for important chemical reactions. Cross-training for students in both the chemical sciences and software development will be provided, preparing them for the STEM workforce. This proposal will also introduce computational chemistry to high school and undergraduate students through a hands-on Instant Supercomputer workshop featuring the construction of a temporary supercomputer.Orland, Overbey and workers investigate chemical reactivity enhancements originating from ionic fluids and to develop new advances in QM/MM methodology. The objective is use QM/MM simulations to resolve controversies regarding the influence of ionic liquids and DES upon rate accelerations, mechanisms, and %ee enhancements when compared to conventional solvents. Development of force field parameters is proposed for multiple choline chloride based DES solvents and 1-alkyl-3-methylimidazolium based ionic liquids. In addition, the creation of a highly parallel, open source software package for performing QM/MM calculations will be made freely available to the scientific simulation community.