Developing a Molecularly Detailed Theoretical Framework for Predicting the Thermodynamic Properties of Ionic Liquids

mcabe, Clare M.Vanderbilt大学电子液体（ILs）是一种完全由复杂离子组成的液体，通常熔点在室温或低于室温，与高温熔盐（如NaCl）区别开来。每种阳离子和阴离子赋予IL不同的物理和化学性质，使IL能够定制以提供所需的性质。虽然最初对il的兴趣主要集中在它们作为溶剂的用途上，但随着il在催化、分离、传感器、太阳能电池、电池、热流体和润滑剂等领域的应用，它的应用范围急剧扩大。这些应用，再加上估计可能达到数十亿的人工智能数量，突显出需要开发一种精确的工具来设计特定任务的人工智能。尽管增加了实验研究和物理性质调查，但目前还不可能预测哪种离子组合将导致所需的一组性质。迄今为止，IL设计的有限进展主要是通过化学成分的实验来实现的，这导致了化学与性能之间的经验启发。尽管具有明显的实用性，但基于对il内部结构和相互作用的深刻物理理解的il预测设计方法目前尚不存在。这部分是因为IL及其与其他分子种类的混合物是非常复杂的系统，从模拟和理论的角度来看，都提出了特别困难的分子建模挑战，特别是如果我们希望能够在缺乏实验数据的情况下预测IL的性质。我们将通过发展基于分子的理论框架来研究il的热力学性质来解决这一需求。所开发的方法将类似于分子模拟研究中使用的模型，并将能够从化学成分中预测IL的性质，从而消除在估计给定离子组合及其与分子物种的混合物的性质时的经验主义。除了能够设计il及其混合物的产品外，拟议的方法将是设计涉及il的化学过程的关键组成部分。

Abstract#1067642McCabe, Clare M.Vanderbilt UniversityIonic liquids (ILs) are liquids, comprised entirely of complex ions, that typically have melting points at or below room temperature, distinguishing them from high temperature molten salts (e.g., NaCl). The cations and anions each impart different physical and chemical properties to the IL enabling ILs to be tailored to provide desired properties. While initial interest in ILs focused on their use as solvents, it has since broadened dramatically with ILs finding applications from catalysis, separations, sensors, solar cells, batteries, thermal fluids and lubricants. These applications, combined with the number of possible ILs being estimated to be in the billions, underlines the need to develop an accurate tool to design task-specific ILs.Despite increased experimental studies and physical property investigations, it is currently not possible to predict which ion combinations will lead to a desired set of properties. The limited progress to date in IL design has been achieved primarily through experimentation in chemical composition leading to empirical heuristics relating chemistry to properties.Despite its obvious utility, a predictive design methodology for ILs, based upon a deep physical understanding of the structure and interactions within ILs, does not exist today. This is in part because ILs and their mixtures with other molecular species are exceptionally complex systems and present particularly difficult molecular modeling challenges, both from simulation and theory points of view, especially if we wish to be able to predict IL properties in the absence of experimental data. We will address this need through the development of a molecular-based theoretical framework with which to study the thermodynamic properties of ILs. The approach developed will be akin to the models used in molecular simulation studies and will enable the prediction of IL properties from the chemical composition, so eliminating empiricism in estimating the properties of a given combination of ions and their mixtures with molecular species. In addition to enabling product design for ILs and their mixtures, the proposed methodology will be a crucial component in the design of chemical processes involving ILs.