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

Stephanie Spittle; Derrick Poe; Brian Doherty; Charles Kolodziej; Luke Heroux; Md Ashraful Haque; Henry Squire; Tyler Cosby; Yong Zhang; Carla Fraenza; Sahana Bhattacharyya; Madhusudan Tyagi; Jing Peng; Ramez A. Elgammal; Thomas Zawodzinski; Mark Tuckerman; Steve Greenbaum; Burcu Gurkan; Mark Dadmun; Edward J. Maginn; Joshua Sangoro

doi:10.1038/s41467-021-27842-z

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

Stephanie Spittle, Derrick Poe, Brian Doherty, Charles Kolodziej, Luke Heroux, Md Ashraful Haque, Henry Squire, Tyler Cosby, Yong Zhang, Carla Fraenza, Sahana Bhattacharyya, Madhusudan Tyagi, Jing Peng, Ramez A. Elgammal, Thomas Zawodzinski, Mark Tuckerman, Steve Greenbaum, Burcu Gurkan, Mark Dadmun, Edward J. MaginnJoshua Sangoro

Chemistry

Research output: Contribution to journal › Article › peer-review

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 ethylene glycol and result in new dynamic modes that are strongly correlated to the macroscopic properties of the DES formed.

Original language	English (US)
Article number	219
Journal	Nature communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-27842-z
State	Published - Dec 2022

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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Spittle, S., Poe, D., Doherty, B., Kolodziej, C., Heroux, L., Haque, M. A., Squire, H., Cosby, T., Zhang, Y., Fraenza, C., Bhattacharyya, S., Tyagi, M., Peng, J., Elgammal, R. A., Zawodzinski, T., Tuckerman, M., Greenbaum, S., Gurkan, B., Dadmun, M., ... Sangoro, J. (2022). Evolution of microscopic heterogeneity and dynamics in choline chloride-based deep eutectic solvents. Nature communications, 13(1), Article 219. https://doi.org/10.1038/s41467-021-27842-z

Spittle, S, Poe, D, Doherty, B, Kolodziej, C, Heroux, L, Haque, MA, Squire, H, Cosby, T, Zhang, Y, Fraenza, C, Bhattacharyya, S, Tyagi, M, Peng, J, Elgammal, RA, Zawodzinski, T, Tuckerman, M, Greenbaum, S, Gurkan, B, Dadmun, M, Maginn, EJ & Sangoro, J 2022, 'Evolution of microscopic heterogeneity and dynamics in choline chloride-based deep eutectic solvents', Nature communications, vol. 13, no. 1, 219. https://doi.org/10.1038/s41467-021-27842-z

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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 ethylene glycol and result in new dynamic modes that are strongly correlated to the macroscopic properties of the DES formed.",

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AU - Haque, Md Ashraful

AU - Squire, Henry

AU - Cosby, Tyler

AU - Zhang, Yong

AU - Fraenza, Carla

AU - Bhattacharyya, Sahana

AU - Tyagi, Madhusudan

AU - Peng, Jing

AU - Elgammal, Ramez A.

AU - Zawodzinski, Thomas

AU - Tuckerman, Mark

AU - Greenbaum, Steve

AU - Gurkan, Burcu

AU - Dadmun, Mark

AU - Maginn, Edward J.

AU - Sangoro, Joshua

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AB - 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 ethylene glycol and result in new dynamic modes that are strongly correlated to the macroscopic properties of the DES formed.

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

Abstract

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