Nasicon-Type Surface Functional Modification in Core–Shell LiNi_0.5Mn_0.3Co_0.2O₂@NaTi₂(PO₄)₃ Cathode Enhances Its High-Voltage Cycling Stability and Rate Capacity toward Li-Ion Batteries

Abstract

Surface modifications are established well as efficient methodologies to enhance comprehensive Li-storage behaviors of the cathodes and play a significant role in cutting edge innovations toward lithium-ion batteries (LIBs). Herein, we first logically devised a pilot-scale coating strategy to integrate solid-state electrolyte NaTi₂(PO₄)₃ (NTP) and layered LiNi_0.5Mn_0.3Co_0.2O₂ (NMC) for smart construction of core-shell NMC@NTP cathodes. The Nasicon-type NTP nanoshell with exceptional ion conductivity effectively suppressed gradual encroachment and/or loss of electroactive NMC, guaranteed stable phase interfaces, and meanwhile rendered small sur-/interfacial electron/ion-diffusion resistance. By benefiting from immanently promoting contributions of the nano-NTP coating, the as-fabricated core-shell NMC@NTP architectures were competitively endowed with superior high-voltage cyclic stabilities and rate capacities within larger electrochemical window from 3.0 to 4.6 V when utilized as advanced cathodes for advanced LIBs. More meaningfully, the appealing electrode design concept proposed here will exert significant impact upon further constructing other high-voltage Ni-based cathodes for high-energy/power LIBs.