LLCZN/PEO/LiPF₆ Composite Solid-State Electrolyte for Safe Energy Storage Application

All-solid-state batteries (ASSBs) are gaining traction in the arena of energy storage due to their promising results in producing high energy density and long cycle life coupled with their capability of being safe. The key challenges facing ASSBs are low conductivity and slow charge transfer kinetics at the interface between the electrode and the solid electrolyte. Garnet solid-state electrolyte has shown promising results in improving the ion conductivity but still suffers from poor capacity retention and rate performance due to the interfacial resistance between the electrodes. To improve the interfacial resistance, we prepared a composite consisting of Li7La2.75Ca0.25Zr1.75Nb0.25O12 (LLCZN) garnet material as the ceramic, polyethylene oxide (PEO) as the polymer, and lithium hexafluorophosphate (LiPF6) as the salt. These compounds are mixed in a stoichiometric ratio and developed into a very thin disc-shaped solid electrolyte. The LLCZN provides a lithium-ion transport path to enhance the lithium-ion conduction during charging and discharging cycles, while the LiPF6 contributes more lithium ions via the transport path. The PEO matrix in the composite material aids in bonding the compounds together and creating a large contact area, thereby reducing the issue of large interfacial resistance. FESEM images show the porous nature of the electrolyte which promotes the movement of lithium ions through the electrolyte. The fabricated LLCZN/PEO/LiPF6 solid-state electrolyte shows outstanding electrochemical stability that remains at 130 mAh g−1 up to 150 charging and discharging cycles at 0.05 mA cm−2 current. All the specific capacities were calculated based on the mass of the cathode material (LiCoO2). In addition, the coin cell retains 85% discharge capacity up to 150 cycles with a Coulombic efficiency of approximately 98% and energy efficiency of 90% during the entire cycling process