Evolution of microscopic heterogeneity and dynamics in choline chloride-based deep eutectic solvents

Authors

Stephanie Spittle, University of Tennessee, Knoxville
Derrick Poe, University of Notre Dame
Brain Doherty, New York University
Charles Kolodziej, Case Western Reserve University
Luke Heroux, University of Tennessee, Knoxville
Md Ashraful Haque, University of Tennessee, Knoxville
Henry Squire, Case Western Reserve University
Tyler Cosby, University of Tennessee Southern
Yong Zhang, University of Notre Dame
Carla Fraenza, CUNY Hunter CollegeFollow
Sahana Bhattacharyya, CUNY Hunter CollegeFollow
Madhusudan Tyagi, University of Maryland
Jing Peng, Beihang University
Ramez A. Elgammal, University of Tennessee, Knoxville
Thomas Zawodzinski, University of Tennessee, Knoxville
Mark Tuckerman, New York University
Steve Greenbaum, CUNY Hunter CollegeFollow
Burcu Gurkan, Case Western Reserve University
Clemens Burda, Case Western Reserve University
Mark Dadmun, University of Tennessee, Knoxville
Edward J. Maginn, University of Notre Dame
Joshua Sangoro, University of Tennessee, Knoxville

Document Type

Article

Publication Date

1-11-2022

Abstract

Deep eutectic solvents (DESs) are an emerging class of non-aqueous solvents that are potentially scalable, easy to prepare and functionalize for many applications ranging from biomass processing to energy storage technologies. Predictive understanding of the fundamental correlations between local structure and macroscopic properties is needed to exploit the large design space and tunability of DESs for specific applications. Here, we employ a range of computational and experimental techniques that span length-scales from molecular to macroscopic and timescales from picoseconds to seconds to study the evolution of structure and dynamics in model DESs, namely Glyceline and Ethaline, starting from the parent compounds. We show that systematic addition of choline chloride leads to microscopic heterogeneities that alter the primary structural relaxation in glycerol and ethyleneglycol and result in new dynamic modes that are strongly correlated to the macroscopic properties of the DES formed.

Comments

This article was originally published in nature communications and can be accessed at https://doi.org/10.1038/s41467-021-27842-z.

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