First-principles modeling of chemistry in mixed solvents: Where to go from here?
First-principles modeling of chemistry in mixed solvents: Where to go from here?
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DOI：
10.1063/1.5143207
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发表时间：
2020-04
期刊：
影响因子：
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通讯作者：
Alex M. Maldonado;Yasemin Basdogan;J. T. Berryman;S. Rempe;J. Keith
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文献类型：
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作者：
Alex M. Maldonado;Yasemin Basdogan;J. T. Berryman;S. Rempe;J. Keith
混合溶剂（即，离子或非离子液体的二元或更高级混合物）在化学合成、分离和电化学装置中起关键作用，因为它们可以针对特定反应和应用进行调整。除了完全明确的溶剂化处理，可能是难以参数化或计算昂贵，目前还没有建立良好的第一原理方案，可靠地模拟原子尺度的化学混合溶剂环境。我们提供了我们的观点，如何在不久的将来实现这一过程的混合溶剂系统变得更加探索使用理论和计算化学。我们首先概述是什么使混合溶剂系统比单组分溶剂复杂得多。概述了目前和有前途的技术建模混合溶剂环境。我们专注于所谓的混合溶剂化处理，如导体样筛选模型的真实的溶剂和参考相互作用网站模型，这是远远低于计算要求比明确的模拟。我们还建议，集群连续的方法植根于物理上严格的准化学理论提供了一个强大的，但实际的，研究混合溶剂中的化学过程的路线。
Mixed solvents (i.e., binary or higher order mixtures of ionic or nonionic liquids) play crucial roles in chemical syntheses, separations, and electrochemical devices because they can be tuned for specific reactions and applications. Apart from fully explicit solvation treatments that can be difficult to parameterize or computationally expensive, there is currently no well-established first-principles regimen for reliably modeling atomic-scale chemistry in mixed solvent environments. We offer our perspective on how this process could be achieved in the near future as mixed solvent systems become more explored using theoretical and computational chemistry. We first outline what makes mixed solvent systems far more complex compared to single-component solvents. An overview of current and promising techniques for modeling mixed solvent environments is provided. We focus on so-called hybrid solvation treatments such as the conductor-like screening model for real solvents and the reference interaction site model, which are far less computationally demanding than explicit simulations. We also propose that cluster-continuum approaches rooted in physically rigorous quasi-chemical theory provide a robust, yet practical, route for studying chemical processes in mixed solvents.