Sandwiching polymer interlayers between the electrode
and solid
electrolyte is considered promising in solving the interfacial issues
arising from solid–solid contact in garnet-based solid-state
batteries, but drawbacks including low ionic conductivity, inferior
Li+ transference number, and unsatisfying mechanical property
of the polymer hindered the practical application of such strategy.
To solve the mentioned shortcomings of the polymer interlayer simultaneously,
we introduce the ferroelectric material, BaTi2O5 (BT) nanorods, into the polymer matrix in this work. By taking full
advantage of the plasticization effect and intrinsic spontaneous polarization
of the introduced ferroelectric, the polymer’s ionic conductivity
and Li+ transference number have been significantly enhanced.
The built-in electric field BT introduced also benefits the modulation
of CEI components formed on the cathode particles, further enhancing
the battery performance by decreasing cathode degradation. Besides,
the BT nanorods’ particular high aspect ratio also helps increase
the mechanical property of the obtained polymer film, making it more
resistant to lithium dendrite growth across the interface. Benefitting
from the merits mentioned above, the assembled lithium symmetric cells
using garnet SE with the BT-modified polymer interlayer exhibit stable
cycling performance (no short circuit after 1000 h under RT) with
low polarization voltage. The full battery employing LiFePO4 as a cathode also presents superior capacity retentions (94.6% after
200 cycles at 0.1 C and 93.4% after 400 cycles at 0.2 C). This work
highlights the importance of ferroelectric materials with specific
morphology in enhancing the electrochemical performance of polymer-based
electrolytes, promoting the practical application of solid-state batteries.