Promoted Stability and Reaction Kinetics in Ni-Rich Cathodes via Mechanical Fusing Multifunctional LiZr(PO) Nanocrystals for High Mass Loading All-Solid-State Lithium Batteries.

Sulfide all-solid-state lithium battery (ASSLB) with nickel-rich layered oxide as the cathode is promising for next-generation energy storage system. However, the Li transport dynamic and stability in ASSLB are hindered by the structural mismatches and the instabilities especially at the oxide cathode/sulfide solid electrolyte (SE) interface. In this work, we have demonstrated a simple and highly effective solid-state mechanofusion method (1500 rpm for 10 min) to combine lithium conductive NASICON-type LiZr(PO) nanocrystals (∼20 nm) uniformly and compactly onto the surface of the single crystallized LiNiCoMnO, which can also attractively achieve Zr doping in NCM811 and oxygen vacancies in the LZPO coating without solvent and annealing. Benefiting from the alleviated interface mismatches, sufficient Li ion flux through the LZPO coating, promoted structural stabilities for both NCM811 and sulfide SE, strong electronic coupling effect between the LZPO and NCM811, and enlarged (003) -spacing with enriched Li migration channels in NCM811, the obtained LZPO-NCM811 exhibits superior stability (185 mAh/g at 0.1C for 200 cycles) and rate performance (105 mAh/g at 1C for 1300 cycles) with high mass loading of 27 mg/cm in sulfide ASSLB. Even with a pronounced 54 mg/cm, LZPO-NCM811 manifests a high areal capacity of 9.85 mAh/cm. The convenient and highly effective interface engineering strategy paves the way to large-scale production of various coated cathode materials with synergistic effects for high performance ASSLBs.