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Polymer Dynamics in Block Copolymer Electrolytes Detected by Neutron Spin Echo

  • Whitney S. Loo
    Whitney S. Loo
    Department of Chemical and Biomolecular Engineering, University of California−Berkeley, Berkeley, California 94720, United States
  • Antonio Faraone
    Antonio Faraone
    National Institute of Standards and Technology Center for Neutron Research, Gaithersburg, Maryland 20899, United States
  • Lorena S. Grundy
    Lorena S. Grundy
    Department of Chemical and Biomolecular Engineering, University of California−Berkeley, Berkeley, California 94720, United States
  • Kevin W. Gao
    Kevin W. Gao
    Department of Chemical and Biomolecular Engineering, University of California−Berkeley, Berkeley, California 94720, United States
    More by Kevin W. Gao
  • , and 
  • Nitash P. Balsara*
    Nitash P. Balsara
    Department of Chemical and Biomolecular Engineering, University of California−Berkeley, Berkeley, California 94720, United States
    Materials Sciences Division  and  Joint Center for Energy Storage Research (JCESR), Lawrence Berkeley National Lab, Berkeley, California 94720, United States
    *E-mail: [email protected]
Cite this: ACS Macro Lett. 2020, 9, 5, 639–645
Publication Date (Web):April 15, 2020
https://doi.org/10.1021/acsmacrolett.0c00236
Copyright © 2020 American Chemical Society

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    Abstract

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    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.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsmacrolett.0c00236.

    • Detailed information on polymer synthesis, quantitative analysis of the scattering experiments, results of fitting procedures shown in Figure 2, and reproduced data on PEO/LiTFSI for direct comparison from refs (15and40) (PDF)

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    Cited By

    This article is cited by 10 publications.

    1. Priyanka M. Ketkar, Nicholas F. Pietra, Andrew G. Korovich, Louis A. Madsen, Thomas H. Epps, III. Role of Intra-Domain Heterogeneity on Ion and Polymer Dynamics in Block Polymer Electrolytes: An Approach for Spatially Resolving Dynamics and Ion Transport. Macromolecules 2023, 56 (21) , 8404-8416. https://doi.org/10.1021/acs.macromol.3c00926
    2. Sheetal K. Jain, Dakota Rawlings, Ségolène Antoine, Rachel A. Segalman, Songi Han. Confinement Promotes Hydrogen Bond Network Formation and Grotthuss Proton Hopping in Ion-Conducting Block Copolymers. Macromolecules 2022, 55 (2) , 615-622. https://doi.org/10.1021/acs.macromol.1c01808
    3. Priyanka M. Ketkar, Thomas H. Epps, III. Nanostructured Block Polymer Electrolytes: Tailoring Self-Assembly to Unlock the Potential in Lithium-Ion Batteries. Accounts of Chemical Research 2021, 54 (23) , 4342-4353. https://doi.org/10.1021/acs.accounts.1c00468
    4. Priyanka M. Ketkar, Kuan-Hsuan Shen, Mengdi Fan, Lisa M. Hall, Thomas H. Epps, III. Quantifying the Effects of Monomer Segment Distributions on Ion Transport in Tapered Block Polymer Electrolytes. Macromolecules 2021, 54 (16) , 7590-7602. https://doi.org/10.1021/acs.macromol.1c00941
    5. Jacqueline A. Maslyn, Louise Frenck, Vijay D. Veeraraghavan, Alexander Müller, Alec S. Ho, Nandan Marwaha, Whitney S. Loo, Dilworth Y. Parkinson, Andrew M. Minor, Nitash P. Balsara. Limiting Current in Nanostructured Block Copolymer Electrolytes. Macromolecules 2021, 54 (9) , 4010-4022. https://doi.org/10.1021/acs.macromol.1c00425
    6. Kuan-Hsuan Shen, Lisa M. Hall. Effects of Ion Size and Dielectric Constant on Ion Transport and Transference Number in Polymer Electrolytes. Macromolecules 2020, 53 (22) , 10086-10096. https://doi.org/10.1021/acs.macromol.0c02161
    7. Jean-Sebastien Benas, Fang-Cheng Liang, Wei-Cheng Chen, Chung-Wei Hung, Jung-Yao Chen, Ye Zhou, Su-Ting Han, Redouane Borsali, Chi-Ching Kuo. Lewis adduct approach for self-assembled block copolymer perovskite quantum dots composite toward optoelectronic application: Challenges and prospects. Chemical Engineering Journal 2022, 431 , 133701. https://doi.org/10.1016/j.cej.2021.133701
    8. Alexander Mayer, Dominik Steinle, Stefano Passerini, Dominic Bresser. Block copolymers as (single-ion conducting) lithium battery electrolytes. Nanotechnology 2022, 33 (6) , 062002. https://doi.org/10.1088/1361-6528/ac2e21
    9. Peter Bennington, Chuting Deng, Daniel Sharon, Michael A. Webb, Juan J. de Pablo, Paul F. Nealey, Shrayesh N. Patel. Role of solvation site segmental dynamics on ion transport in ethylene-oxide based side-chain polymer electrolytes. Journal of Materials Chemistry A 2021, 9 (15) , 9937-9951. https://doi.org/10.1039/D1TA00899D
    10. Avneesh Kumar. Cooperative proton conduction in sulfonated and phosphonated hybrid random copolymers. Journal of Materials Chemistry A 2020, 8 (43) , 22632-22636. https://doi.org/10.1039/D0TA07732A

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