Nanosecond solvation dynamics in a polymer electrolyte for lithium batteries

Neel J. Shah; Chao Fang; Naresh C. Osti; Eugene Mamontov; Xiaopeng Yu; Jaeyong Lee; Hiroshi Watanabe; Rui Wang; Nitash P. Balsara

doi:10.1038/s41563-024-01834-y

Nanosecond solvation dynamics in a polymer electrolyte for lithium batteries

Neel J. Shah, Chao Fang, Naresh C. Osti, Eugene Mamontov, Xiaopeng Yu, Jaeyong Lee, Hiroshi Watanabe, Rui Wang, Nitash P. Balsara

Chemical Spectroscopy

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6 Scopus citations

Abstract

Solvation dynamics critically affect charge transport. Spectroscopic experiments and computer simulations show that these dynamics in aqueous systems occur on a picosecond timescale. In the case of organic electrolytes, however, conflicting values ranging from 1 to several 100 picoseconds have been reported. We resolve this conflict by studying mixtures of an organic polymer and a lithium salt. Lithium ions coordinate with multiple polymer chains, resulting in temporary crosslinks. Relaxation of these crosslinks, detected by quasielastic neutron scattering, are directly related to solvation dynamics. Simulations reveal a broad spectrum of relaxation times. The average timescale for solvation dynamics in both experiment and simulation is one nanosecond. We present the direct measurement of ultraslow dynamics of solvation shell break-up in an electrolyte.

Original language	English
Pages (from-to)	664-669
Number of pages	6
Journal	Nature Materials
Volume	23
Issue number	5
DOIs	https://doi.org/10.1038/s41563-024-01834-y
State	Published - May 2024

Funding

This work was supported by the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the US Department of Energy, Office of Science, Office of Basic Energy Science, under contract no. DE-AC02-06CH11357. This research used resources at the Spallation Neutron Source, a US Department of Energy, Office of Science User Facility operated by Oak Ridge National Laboratory. The computations were performed at the Lawrencium cluster at Lawrence Berkeley National Laboratory.

Funders	Funder number
Joint Center for Energy Storage Research
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC02-06CH11357

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10.1038/s41563-024-01834-y

Cite this

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AU - Watanabe, Hiroshi

AU - Wang, Rui

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Nanosecond solvation dynamics in a polymer electrolyte for lithium batteries

Abstract

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