Anion chemical composition of poly(ethylene oxide)-based sulfonylimide and sulfonate lithium ionomers controls ion aggregation and conduction

Mei, Wenwen; Yu, Deyang; George, Christy; Madsen, Louis A.; Hickey, Robert J.; Colby, Ralph H.

doi:10.1039/d2tc02212e

Title: Anion chemical composition of poly(ethylene oxide)-based sulfonylimide and sulfonate lithium ionomers controls ion aggregation and conduction

Journal Article · 01 September 2022 · Journal of Materials Chemistry C

DOI: https://doi.org/10.1039/d2tc02212e · OSTI ID:2425452

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^[2]; George, Christy ^[1];

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Pennsylvania State Univ., University Park, PA (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

Maximizing ion conduction in single-ion-conducting ionomers is essential for their application in energy-related technologies such as Li-ion batteries. Understanding the anion chemical composition impacts on ion conduction offers new perspectives to maximize ion transport, since the current approach of lowering T_g has apparently reached a limit (lowest T_g ~ 190 K, highest conductivity ~10^-5–10^-4 S cm^-1). Here, a series of random ionomers are synthesized by copolymerizing poly(ethylene glycol)methacrylate with either sulfonylimide lithium methacrylate (MTLi) or sulfonate lithium methacrylate (MSLi) using reversible addition–fragmentation chain transfer (RAFT) polymerization. Li-Ion conduction and self-diffusion coefficients (DLi+) of the ionomers are characterized with dielectric relaxation spectroscopy (DRS) and pulsed-field-gradient (PFG) NMR diffusometry, respectively. Increasing ion content decreases the Li-ion conductivity and D_Li+, as expected from the increased T_g. Moreover, a considerably lower ionic conductivity and D_Li+ are observed for MSLi compared to MTLi at constant ion content and T_g/T. As revealed from X-ray scattering, strong ion aggregation in MSLi results in much lower conductivity and DLi+ compared with less aggregated MTLi based on the more delocalized sulfonylimide anion. These results emphasize the detrimental and molecularly specific role of ion aggregation in Li-ion conductivity, and highlight the necessity for minimizing ion aggregation via the rational choice of anion chemical composition.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2425452

Journal Information:: Journal of Materials Chemistry C, Journal Name: Journal of Materials Chemistry C Journal Issue: 39 Vol. 10; ISSN JMCCCX; ISSN 2050-7526

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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