Achieving Uniform Ti/P Co‐Modifications for Optimized Li + Transport Kinetics of LiCoO 2

Abstract Recently, the deteriorated Li + transport kinetics of LiCoO 2 (LCO) due to the presence of uneven surface coatings and dopants has long puzzled researchers. Herein, by using the hydrolysis of tetrabutyl titanate (C 16 H 36 O 4 Ti), the interaction between LCO and LiH 2 PO 4 is effectively regulated, constructing uniform Li 3 PO 4 deposit and Ti‐enriched rocksalt (RS) phase on the surface of TP‐LCO. The ultrathin Ti‐enriched RS phase can effectively stabliize the surface lattice oxygen and enhance Li + transport kinetics, suppressing the Co/O loss and structural collapse. Simultaneously, the uniformly distributed Li 3 PO 4 deposits serve as a substrate that facilitates the formation of the reinforced and P‐enriched cathode‐electrolyte interphase (CEI), ensuring the long‐term cycling structural stability. Benefiting from the synergistic effect of uniform bilayer structure, TP‐LCO presents a high capacity of 181.7 mA h g −1 at the current of 8 C in the TP‐LCO/Li cell, and a high capacity retention of 90.9% after 600 cycles at the current of 1 C in the TP‐LCO/graphite cell.