Abstract
Sulfide-based solid-state batteries (SSBs) are emerging as a top contender for next-generation rechargeable batteries with improved safety and higher energy densities. However, SSBs with Ni-rich cathode materials such as LiNi(0.82)Mn(0.07)Co(0.11)O(2) (NMC82) exhibit several chemomechanical challenges at the cathode-electrolyte interface, such as contact loss and solid-electrolyte decomposition, resulting in poor interfacial Li(+) ion transport. To overcome these challenges, we used polymerized ionic liquids (PIL) as coatings at the NMC82 cathode surface, with and without incorporating a lithium salt. The thin Li(+) ion-conductive Li-PIL nanocoating shows excellent compatibility with sulfide solid electrolytes and enables efficient Li(+) transfer over the cathode-solid electrolyte interface, as demonstrated by 2D solid-state exchange NMR. It also improves contact retention between the cathode-solid electrolyte particles and mitigates electrolyte oxidation-induced degradation. This is reflected in the electrochemical performance of coated NMC82 in sulfide SSBs, where both a higher rate performance (190 mA h g(-1) vs. 163 mA h g(-1) for uncoated at 0.1C) and a remarkable capacity retention of 82.7% after 500 cycles at 0.2C and ambient conditions (20 °C) are observed. These results emphasize the effectiveness of PILs with Li salts as multifunctional coatings that enable high-performance sulfide-based SSBs with Ni-rich cathode materials at ambient temperature.