A critical challenge in the commercialization of layer-structured Ni-rich materials is the fast capacity drop and voltage fading due to the interfacial instability and bulk structural degradation of the cathodes during battery operation. Herein, with the guidance of theoretical calculations of migration energy difference between La and Ti from the surface to the inside of LiNi 0.8 Co 0.1 Mn 0.1 O 2 , for the first time, Ti-doped and La 4 NiLiO 8 -coated LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes are rationally designed and prepared, via a simple and convenient dual-modification strategy of synchronous synthesis and in situ modification. Impressively, the dual modified materials show remarkably improved electrochemical performance and largely suppressed voltage fading, even under exertive operational conditions at elevated temperature and under extended cutoff voltage. Further studies reveal that the nanoscale structural degradation on material surfaces and the appearance of intergranular cracks associated with the inconsistent evolution of structural degradation at the particle level can be effectively suppressed by the synergetic effect of the conductive La 4 NiLiO 8 coating layer and the strong TiO bond. The present work demonstrates that our strategy can simultaneously address the two issues with respect to interfacial instability and bulk structural degradation, and it represents a significant progress in the development of advanced cathode materials for high-performance lithium-ion batteries.

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Although LiNi 0.8 Co 0.1 Mn 0.1 O 2 is attracting increasing attention on account of its high specific capacity, the moderate cycle lifetime still hinders its large-scale commercialization applications. Herein, the Ti-doped LiNi 0.8 Co 0.1 Mn 0.1 O 2 compounds are successfully synthesized. The Li(Ni 0.8 Co 0.1 Mn 0.1 ) 0.99 Ti 0.01 O 2 sample exhibits the best electrochemical performance. Under the voltage range of 2.7 – 4.3 V, it maintains a reversible capacity of 151.01 mAh·g −1 with the capacity retention of 83.98% after 200 cycles at 1 C. Electrochemical impedance spectroscopy (EIS) and differential capacity profiles during prolonged cycling demonstrate that the Ti doping could enhance both the abilities of electronic transition and Li ion diffusion. More importantly, Ti doping can also improve the reversibility of the H2-H3 phase transitions during charge-discharge cycles, thus improving the electrochemical performance of Ni-rich cathodes.

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