Lithium Borate Polycarbonates for High-Capacity Solid-State Composite Cathodes.

Improving composite cathode function is key to the success of the solid-state battery. Maximizing attainable cathode capacity and retention requires integrating suitable polymeric binders that retain a sufficiently high ionic conductivity and long-term chemo-mechanical stability of the cathode active material-solid-electrolyte-carbon mixture. Herein, we report block copolymer networks composed of lithium borate polycarbonates and poly(ethylene oxide) that improved the capacity (200 mAh g -1 at 1.75 mA cm -2 ) and capacity retention (94 % over 300 cycles) of all-solid-state composite cathodes with nickel-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode active material, Li 6 PS 5 Cl solid electrolyte, and carbon. Tetrahedral B(OR) 2 (OH) 2 - anions immobilized on the polycarbonate segments provide hydrogen-bonding chain crosslinking and selective Li-counterion conductivity, parameterized by Li-ion transference numbers close to unity (t Li+ ~0.94). With 90 wt % polycarbonate content and a flexible low glass transition temperature backbone, the single-ion conductors achieved high Li-ion conductivities of 0.2 mS cm -1 at 30 °C. The work should inform future binder design for improving the processability of cathode composites towards commercializing solid-state batteries, and allow use in other cell configurations, such as lithium-sulphur cathode designs.