Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 11, Pages 13196-13205Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c21853
Keywords
lithium-metal battery; ionic liquids; SEI modification; Ni-rich cathode; degradation mechanism
Funding
- Australian Research Council (ARC) through the ARC Training Centre for Future Energy Storage Technologies [IC180100049]
- Office of the Deputy Vice-Chancellor of Research of Deakin University through the Battery Technology Research and Innovation Hub (BatTRI-Hub)
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This study investigated the use of highly concentrated ionic liquid electrolyte for high-voltage Ni-rich cathodes, achieving a stable electrode/electrolyte interface and efficient long-term cycling performance.
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 (C(3)mpyrFSI) 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 degrees C. Fitting of acquired impedance spectra indicated that the SEI resistivity (R-SEI) 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 (R-CT) throughout cycling.
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