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Title: Polymer Dynamics in Block Copolymer Electrolytes Detected by Neutron Spin Echo

Abstract

Polymer chain dynamics of a nanostructured block copolymer electrolyte, polystyrene-block-poly(ethylene oxide) (SEO) mixed with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, are investigated by neutron spin echo (NSE) spectroscopy on the 0.1–100 ns time scale and analyzed using the Rouse model at short times (t ≤ 10 ns) and the reptation tube model at long times (t ≥ 50 ns). In the Rouse regime, the monomeric friction coefficient increases with increasing salt concentration, as seen previously in homopolymer electrolytes. In the reptation regime, the tube diameters, which represent entanglement constraints, decrease with increasing salt concentration. The normalized longest molecular relaxation time, calculated from the NSE results, increases with increasing salt concentration. We argue that quantifying chain motion in the presence of ions is essential for predicting the behavior of polymer-electrolyte-based batteries operating at large currents.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
  3. Univ. of California, Berkeley, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institute of Standards and Technology (NIST); US Department of Commerce; National Science Foundation (NSF)
OSTI Identifier:
1633251
Grant/Contract Number:  
AC02-05CH11231; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Macro Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 5; Journal ID: ISSN 2161-1653
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Salts; Batteries; Electrolytes; Polymers; Copolymers

Citation Formats

Loo, Whitney S., Faraone, Antonio, Grundy, Lorena S., Gao, Kevin W., and Balsara, Nitash P. Polymer Dynamics in Block Copolymer Electrolytes Detected by Neutron Spin Echo. United States: N. p., 2020. Web. doi:10.1021/acsmacrolett.0c00236.
Loo, Whitney S., Faraone, Antonio, Grundy, Lorena S., Gao, Kevin W., & Balsara, Nitash P. Polymer Dynamics in Block Copolymer Electrolytes Detected by Neutron Spin Echo. United States. https://doi.org/10.1021/acsmacrolett.0c00236
Loo, Whitney S., Faraone, Antonio, Grundy, Lorena S., Gao, Kevin W., and Balsara, Nitash P. Wed . "Polymer Dynamics in Block Copolymer Electrolytes Detected by Neutron Spin Echo". United States. https://doi.org/10.1021/acsmacrolett.0c00236. https://www.osti.gov/servlets/purl/1633251.
@article{osti_1633251,
title = {Polymer Dynamics in Block Copolymer Electrolytes Detected by Neutron Spin Echo},
author = {Loo, Whitney S. and Faraone, Antonio and Grundy, Lorena S. and Gao, Kevin W. and Balsara, Nitash P.},
abstractNote = {Polymer chain dynamics of a nanostructured block copolymer electrolyte, polystyrene-block-poly(ethylene oxide) (SEO) mixed with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, are investigated by neutron spin echo (NSE) spectroscopy on the 0.1–100 ns time scale and analyzed using the Rouse model at short times (t ≤ 10 ns) and the reptation tube model at long times (t ≥ 50 ns). In the Rouse regime, the monomeric friction coefficient increases with increasing salt concentration, as seen previously in homopolymer electrolytes. In the reptation regime, the tube diameters, which represent entanglement constraints, decrease with increasing salt concentration. The normalized longest molecular relaxation time, calculated from the NSE results, increases with increasing salt concentration. We argue that quantifying chain motion in the presence of ions is essential for predicting the behavior of polymer-electrolyte-based batteries operating at large currents.},
doi = {10.1021/acsmacrolett.0c00236},
journal = {ACS Macro Letters},
number = 5,
volume = 9,
place = {United States},
year = {2020},
month = {4}
}

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