In-situ polymerized and crosslinked electrolytes with interchangeable Li/Na transport for battery applications

Singh, Harmandeep; Damron, Josh T.; Shahriar, M.; Danielson, Mary; Beard, Rob; Eberhard, Rachel; Polizos, Georgios; Popov, Ivan; Rahman, Md Anisur; Sokolov, Alexei P.; Gainaru, Catalin

doi:10.20517/energymater.2025.07

In-situ polymerized and crosslinked electrolytes with interchangeable Li/Na transport for battery applications

Journal Article · Tue Sep 30 00:00:00 EDT 2025 · Energy Materials

DOI:https://doi.org/10.20517/energymater.2025.07· OSTI ID:3017027

Singh, Harmandeep ^[1]; Damron, Josh T. ^[2]; Shahriar, M. ^[3]; ^[2]; Beard, Rob ^[2]; Eberhard, Rachel ^[2]; ^[2]; ^[4]; ^[2]; ^[5]; ^[2]

Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Iowa State Univ., Ames, IA (United States)
Univ. of Tennessee, Knoxville, TN (United States). UT-Oak Ridge Innovation Institute (UT-ORII)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

The next generation of batteries requires electrolytes with high conductivity, mechanical stability, good adhesion with electrodes, wide electrochemical windows, and scalability. The present study introduces a concept of doped quasi single-ion conducting copolymers based on methacrylate-(trifluoromethanesulfonyl)imide (TFSI) and vinyl ethylene carbonate which at room temperature are mechanically robust and display ionic conductivities of ~0.1 mS/cm. These electrolytes can be polymerized/crosslinked in-situ, making them easily implementable in current battery manufacturing technologies. They also allow for switching between Li⁺ and Na⁺ transport using simple chemistry procedures. To demonstrate their potential for battery applications, the newly developed Li conductors have been tested in symmetric cells, exhibiting overall impedance below 350 Ohm and plating/stripping stability up to 1 mA/cm². Moreover, lithium metal batteries incorporating this electrolyte and high-voltage Lithium Nickel Manganese Cobalt Oxide (NMC) cathodes show good capacity retention (~79%) during charging and discharging for 80 cycles at C/10 rate and a Coulombic efficiency close to 100% in the entire measurement range. The compositional, mechanical and electrochemical versatility of these electrolytes opens new venues for the design of polymer-based batteries capable of fast charging and extended cycle life, aligning with the current global green energy storage strategies.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 3017027

Journal Information:: Energy Materials, Journal Name: Energy Materials Journal Issue: 12 Vol. 5; ISSN 2770-5900

Publisher:: OAECopyright Statement

Country of Publication:: United States

Language:: English

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