[en] 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.
Research center :
ULHPC - University of Luxembourg: High Performance Computing
Disciplines :
Physical, chemical, mathematical & earth Sciences: Multidisciplinary, general & others
Author, co-author :
Maldonado, Alex; University of Pittsburgh > Department of Chemical and Petroleum Engineering
Basdogan, Yasemin; University of Pittsburgh > Department of Chemical and Petroleum Engineering
Berryman, Josh ; University of Luxembourg > Faculty of Science, Technology and Communication (FSTC) > Physics and Materials Science Research Unit
Rempe, Susan; Sandia National Laboratories > Centre for Computational Biology and Biophysics
Keith, John; University of Pittsburgh > Department of Chemical and Petroleum Engineering
External co-authors :
yes
Language :
English
Title :
First-principles modeling of chemistry in mixed solvents: Where to go from here?
Publication date :
01 April 2020
Journal title :
Journal of Chemical Physics
ISSN :
1089-7690
Publisher :
American Institute of Physics, New York, United States - New York