RESUMO
A set of ionic quasi-block copolymers were investigated to determine the effects of their composition and structure on their performance in their application as solid-state battery electrolytes. Diffusion and electrochemical tests have shown that these new quasi-block electrolytes have comparable performance to traditional block copolymers reaching ionic conductivities of 3.8 × 10-4 S cm-1 and lithium-ion diffusion of 4.6 × 10-12 m2 s-1 at 80 °C. It was illustrated that the mechanical properties of each quasi-block electrolyte are highly dependent on the order of monomer addition in polymer synthesis while the phase morphology hints at each of the quasi-blocks' unique compositional make up.
RESUMO
Employing high-voltage Ni-rich cathodes in Li metal batteries (LMBs) requires stabilization of the electrode/electrolyte interfaces at both electrodes. A stable solid-electrolyte interphase (SEI) and suppression of active material pulverization remain the greatest challenges to achieving efficient long-term cycling. Herein, studies of NMC622 (1 mAh cm-2) cathodes were performed using highly concentrated N-methyl-N-propylpyrrolidinium bis(fluorosulfonyl)imide (C3mpyrFSI) 50 mol % lithium bis(fluorosulfonyl)imide (LiFSI) ionic liquid electrolyte (ILE). The resulting SEI formed at the cathode enabled promising cycling performance (98.13% capacity retention after 100 cycles), and a low degree of ion mixing and lattice expansion was observed, even at an elevated temperature of 50 °C. Fitting of acquired impedance spectra indicated that the SEI resistivity (RSEI) had a low and stable contribution to the internal resistivity of the system, whereas active material pulverization and secondary grain isolation significantly increased the charge transfer resistance (RCT) throughout cycling.
