Stabilizing effects of atomic Ti doping on high-voltage high-nickel layered oxide cathode for lithium-ion rechargeable batteries

High-voltage high-nickel lithium layered oxide cathodes show great application prospects to meet the ever-increasing demand for further improvement of the energy density of rechargeable lithium-ion batteries (LIBs) mainly due to their high output capacity. However, severe bulk structural degradation and undesired electrode-electrolyte interface reactions seriously endanger the cycle life and safety of the battery. Here, 2 mol% Ti atom is used as modified material doping into LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM) to reform LiNi 0.6 Co 0.2 Mn 0.18 Ti 0.02 O 2 (NCM-Ti) and address the long-standing inherent problem. At a high cut-off voltage of 4.5 V, NCM-Ti delivers a higher capacity retention ratio (91.8% vs. 82.9%) after 150 cycles and a superior rate capacity (118 vs. 105 mAh·g-1) at the high current density of 10 C than the pristine NCM. The designed high-voltage full battery with graphite as anode and NCM-Ti as cathode also exhibits high energy density (240 Wh·kg-1) and excellent electrochemical performance. The superior electrochemical behavior can be attributed to the improved stability of the bulk structure and the electrode-electrolyte interface owing to the strong Ti-O bond and no unpaired electrons. The in-situ X-ray diffraction analysis demonstrates that Ti-doping inhibits the undesired H2-H3 phase transition, minimizing the mechanical degradation. The ex-situ TEM and X-ray photoelectron spectroscopy reveal that Ti-doping suppresses the release of interfacial oxygen, reducing undesired interfacial reactions. This work provides a valuable strategic guideline for the application of high-voltage high-nickel cathodes in LIBs.