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

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

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10.1038/s41467-021-27842-z

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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), [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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title = "Evolution of microscopic heterogeneity and dynamics in choline chloride-based deep eutectic solvents",

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.",

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

note = "Funding Information: This work was supported as part of the Breakthrough Electrolytes for Energy Storage (BEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award #: DE-SC0019409. D.P., Y.Z., and E.M. thank the Center for Research Computing (CRC) at the University of Notre Dame for providing computational resources. S.S., T.C., and J.S. thank Yangyang Wang at Oak Ridge National Laboratory for instrument use in the Center for Nanophase Materials Sciences. Access to HFBS was provided by the Center for High Resolution Neutron Scattering, a partnership between the NIST and the National Science Foundation under agreement no. DMR-2010792. The identification of any commercial product or trade name does not imply endorsement or recommendation by NIST. Publisher Copyright: {\textcopyright} 2022, The Author(s).",

year = "2022",

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doi = "10.1038/s41467-021-27842-z",

language = "English (US)",

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AU - Spittle, Stephanie

AU - Poe, Derrick

AU - Doherty, Brian

AU - Kolodziej, Charles

AU - Heroux, Luke

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

N1 - Funding Information: This work was supported as part of the Breakthrough Electrolytes for Energy Storage (BEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award #: DE-SC0019409. D.P., Y.Z., and E.M. thank the Center for Research Computing (CRC) at the University of Notre Dame for providing computational resources. S.S., T.C., and J.S. thank Yangyang Wang at Oak Ridge National Laboratory for instrument use in the Center for Nanophase Materials Sciences. Access to HFBS was provided by the Center for High Resolution Neutron Scattering, a partnership between the NIST and the National Science Foundation under agreement no. DMR-2010792. The identification of any commercial product or trade name does not imply endorsement or recommendation by NIST. Publisher Copyright: © 2022, The Author(s).

PY - 2022/12

Y1 - 2022/12

N2 - 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.

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

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