Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes
Abstract
We report designing new electrolytes requires a better understanding of the correlation between their transport properties and their molecular structure. In this work, we present a detailed study of ionic liquids and polymer gel electrolytes probing their structure and dynamics by nuclear magnetic resonance (NMR) spectroscopy. In particular, ammonium- and phosphonium-based ionic liquids (ILs) are combined with different LiTFSI concentrations, and then with different ratios of poly(methylmethacrylate) polymer. The temperature dependence of self-diffusion coefficients of mobile species, DLi+, DTFSI- and DP4441+ or DN4441+, measured by pulsed field gradient (PFG) NMR spectroscopy obeys the Arrhenius equation. Diffusivity of [P4441][TFSI] ILs is found to be greater than those of the [N4441][TFSI] ILs in both liquid and gel electrolytes. Solid state NMR experiments including 13C and 19F MAS, 13C{19F},13C{1H} CPMAS probe the local structure and molecular-level interactions between ions and polymer in gel electrolytes, particularly for samples with higher PMMA content (≥25 wt%). Finally, the fast field cycling relaxometry has been used to unveil the rotational and translational dynamics of P4441+ or N4441+ and TFSI- by measuring 1H and 19F R1 relaxation rate profiles at different temperatures. A comprehensive NMR analysis including relaxation studies at low magnetic field provides decisive new insights regardingmore »
- Authors:
-
- City Univ. of New York (CUNY), NY (United States)
- New York Structural Biology Center, New York, NY (United States)
- Publication Date:
- Research Org.:
- Case Western Reserve Univ., Cleveland, OH (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Department of the Navy, Office of Naval Research (ONR); National Institutes of Health (NIH)
- OSTI Identifier:
- 1853227
- Alternate Identifier(s):
- OSTI ID: 1776458
- Grant/Contract Number:
- SC0019409; N00014-20-1-2186; CORR015495
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Molecular Liquids
- Additional Journal Information:
- Journal Volume: 329; Journal Issue: C; Journal ID: ISSN 0167-7322
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; ionic liquids; polymer gel electrolytes; PFG NMR; structure and dynamics; solid state NMR; fast field cycling relaxometry
Citation Formats
Garaga, Mounesha N., Jayakody, Nishani, Fraenza, Carla C., Itin, Boris, and Greenbaum, Steven. Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes. United States: N. p., 2021.
Web. doi:10.1016/j.molliq.2021.115454.
Garaga, Mounesha N., Jayakody, Nishani, Fraenza, Carla C., Itin, Boris, & Greenbaum, Steven. Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes. United States. https://doi.org/10.1016/j.molliq.2021.115454
Garaga, Mounesha N., Jayakody, Nishani, Fraenza, Carla C., Itin, Boris, and Greenbaum, Steven. Sat .
"Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes". United States. https://doi.org/10.1016/j.molliq.2021.115454. https://www.osti.gov/servlets/purl/1853227.
@article{osti_1853227,
title = {Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes},
author = {Garaga, Mounesha N. and Jayakody, Nishani and Fraenza, Carla C. and Itin, Boris and Greenbaum, Steven},
abstractNote = {We report designing new electrolytes requires a better understanding of the correlation between their transport properties and their molecular structure. In this work, we present a detailed study of ionic liquids and polymer gel electrolytes probing their structure and dynamics by nuclear magnetic resonance (NMR) spectroscopy. In particular, ammonium- and phosphonium-based ionic liquids (ILs) are combined with different LiTFSI concentrations, and then with different ratios of poly(methylmethacrylate) polymer. The temperature dependence of self-diffusion coefficients of mobile species, DLi+, DTFSI- and DP4441+ or DN4441+, measured by pulsed field gradient (PFG) NMR spectroscopy obeys the Arrhenius equation. Diffusivity of [P4441][TFSI] ILs is found to be greater than those of the [N4441][TFSI] ILs in both liquid and gel electrolytes. Solid state NMR experiments including 13C and 19F MAS, 13C{19F},13C{1H} CPMAS probe the local structure and molecular-level interactions between ions and polymer in gel electrolytes, particularly for samples with higher PMMA content (≥25 wt%). Finally, the fast field cycling relaxometry has been used to unveil the rotational and translational dynamics of P4441+ or N4441+ and TFSI- by measuring 1H and 19F R1 relaxation rate profiles at different temperatures. A comprehensive NMR analysis including relaxation studies at low magnetic field provides decisive new insights regarding the formation of ionic clusters and the interaction of ions with the polymer chain in the case of the gel electrolytes.},
doi = {10.1016/j.molliq.2021.115454},
journal = {Journal of Molecular Liquids},
number = C,
volume = 329,
place = {United States},
year = {Sat Jan 23 00:00:00 EST 2021},
month = {Sat Jan 23 00:00:00 EST 2021}
}
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