Advancing QM/MM Methods to Model Reactions in Ionic Fluids

化学系的化学理论、模型和计算方法(CTMC)计划通过这一奖项资助奥本大学的Orlando Acevedo和Jeffrey Overbey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的计算和数据启用科学与工程(CDS&amp；E)项目为该奖项做出了贡献。由于每年处理的化学废物超过1亿磅，更好地了解如何为化学反应优化可回收溶剂具有潜在的社会影响，从实验室工作台到大规模工业制造。离子液体是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，一种名为深度共熔溶剂(DES)的新离子液体家族最近作为一种环境更安全、相对便宜的替代品而出现。作为化学反应的媒介，每一类溶剂都有明显的优点；然而，DES才刚刚开始成为一种潜在的替代品。目前的研究将有助于建立对离子液体和DES溶剂化整个化学反应过程中发生的分子间相互作用的坚定理解。其策略是使用高端计算模型来阐明这些离子流体对重要化学反应的产物形成机制的影响。将为学生提供化学科学和软件开发方面的交叉培训，为他们进入STEM劳动力做好准备。这项提议还将通过一个以建造临时超级计算机为特色的动手即时超级计算机研讨会向高中生和本科生介绍计算化学。奥兰德、奥弗贝和工作人员研究来自离子液体的化学反应增强，并开发QM/MM方法学的新进展。我们的目标是使用QM/MM模拟来解决与传统溶剂相比，离子液体和DES对速率加速、机理和%ee增强的影响的争议。提出了基于氯化胆碱的DES溶剂和基于1-烷基-3-甲基咪唑的离子液体的力场参数的发展。此外，科学模拟界将免费提供用于执行QM/MM计算的高度并行的开放源码软件包的创建。

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.