Solid-state Li-metal batteries (LMBs) are attracting extensive attention owing to their exceptionally high energy density. Solid electrolytes play a vital role in the practical application of LMBs due to their nonflammable nature and interfacial stability with Li metal, but they ordinarily have a low ionic conductivity and dimensional stability. Here, a selective Li+ conductive solid-state electrolyte (SLCSE) that comprises a highly conductive yet mechanically robust, anion-immobilized (CMA) polymer matrix synthesized by soft-rigid coupled ether-abundant epoxy monomers and branched polyamine, is reported. Rationally incorporated rigid benzene-ring constituents in the CMA matrix not only enhance mechanical strength but also boost Li+ transportation by suppressing crystallinity. The semi-interpenetrating network of the CMA matrix and polyvinylidene fluoride-co-hexafluoropropylene displays synergistic Li+ acceleration behavior by promoting the dissociation and diffusion of Li+ while immobilizing anions, which is elucidated via molecular dynamics simulations. The SLCSE exhibits a high ionic conductivity (3.4 mS cm−1) with a high Li+ transference number (0.77), and SLCSE-based LMBs (Li/SLCSE/LiCoO2 cell) show a high discharge capacity of 146 mAh g−1 (0.2 C) and 126 mAh g−1 (3 C). Furthermore, they show exceptional long cycle stability (90% capacity retention after 500 cycles at 0.5 C), representing remarkable Li dendrite suppression capability.
|Journal||Journal of Membrane Science|
|Publication status||Published - 2023 Feb 15|
Bibliographical noteFunding Information:
J.H.Park acknowledges the support by the Technology Innovation Program (‘ 20013621 ’, Center for Super Critical Material Industrial Technology) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea) . This research was supported by the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT ( 2018M3D1A1058624 , 2019R1A2C3010479 ). This research was also supported by BrainLink program funded by the Ministry of Science and ICT through the National Research Foundation of Korea ( 2022H1D3A3A01077254 ).
© 2022 Elsevier B.V.
All Science Journal Classification (ASJC) codes
- Materials Science(all)
- Physical and Theoretical Chemistry
- Filtration and Separation