Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes

Garaga, Mounesha N.; Jayakody, Nishani; Fraenza, Carla C.; Itin, Boris; Greenbaum, Steven

doi:10.1016/j.molliq.2021.115454

Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes

Journal Article · Fri Jan 22 23:00:00 EST 2021 · Journal of Molecular Liquids

DOI:https://doi.org/10.1016/j.molliq.2021.115454· OSTI ID:1853227

Garaga, Mounesha N. ^[1]; Jayakody, Nishani ^[2]; Fraenza, Carla C. ^[2]; Itin, Boris ^[3]; Greenbaum, Steven ^[2]

City Univ. of New York (CUNY), NY (United States); City Univ. of New York (CUNY), NY (United States)
City Univ. of New York (CUNY), NY (United States)
New York Structural Biology Center, New York, NY (United States)

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, D_Li+, D_TFSI- and D_P4441+ or D_N4441+, 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.

View Accepted Manuscript (DOE)

Research Organization:: Case Western Reserve Univ., Cleveland, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); US Office of Naval Research; National Institutes of Health (NIH)

Grant/Contract Number:: SC0019409

OSTI ID:: 1853227

Alternate ID(s):: OSTI ID: 1776458

Journal Information:: Journal of Molecular Liquids, Journal Name: Journal of Molecular Liquids Journal Issue: C Vol. 329; ISSN 0167-7322

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes

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