Nanosecond solvation dynamics in a polymer electrolyte for lithium batteries

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

doi:10.1038/s41563-024-01834-y

Title: Nanosecond solvation dynamics in a polymer electrolyte for lithium batteries

Journal Article · 26 February 2024 · Nature Materials

DOI: https://doi.org/10.1038/s41563-024-01834-y · OSTI ID:2324006

^[1]; Fang, Chao ^[1];

^[2];

^[2]; Yu, Xiaopeng ^[3];

^[3]; Watanabe, Hiroshi ^[4];

^[1];

^[1]

University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division
Kyoto University, Uji (Japan)

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. Here we present the direct measurement of ultraslow dynamics of solvation shell break-up in an electrolyte.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 2324006

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 4 Vol. 23; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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