Lingua G., Shevtsov V.Y., Vlasov P.S., Puchot L., Gerbaldi C., Shaplov A.S.
ACS Materials Letters, vol. 6, n° 12, pp. 5429-5437, 2024
The choice of ionic-liquid-like monomers (ILM) for single-ion conducting polyelectrolytes (SICPs) is crucial for the performance of all-solid-state lithium batteries. In the current study, we propose a novel approach for development of SICPs via design and synthesis of a new ILM with long poly(ethylene oxide) spacer between methacrylic group and (trifluoromethane)sulfonylimide anion. Its homopolymer shows an ionic conductivity that is ∼5 orders of magnitude higher (9.2 × 10<sup>-8</sup> S cm<sup>-1</sup> at 25 °C), in comparison with previously reported analogues, while the conductivity of its random copolymer with poly(ethylene glycol)methyl ethermethacrylate reaches the levels of 10<sup>-6</sup> and 10<sup>-5</sup> S cm<sup>-1</sup> at 25 and 70 °C, respectively. The copolymer provides excellent thermal (T<sub>onset</sub> ≈ 200 °C) and electrochemical (4.5 V vs Li<sup>+</sup>/Li) stabilities, good compatibility with Li metal, and effective suppression of dendrite growth. Li/SICP/LiFePO<sub>4</sub> cells are capable of reversibly operating at different C rates, demonstrating excellent Coulombic efficiency and retaining specific capacity upon prolonged charge/discharge cycling at a relatively high current rate (C/5) at 70 °C.
