The
Li-rich and Mn-based material xLi2MnO3·(1–x)LiMO2 (M = Ni,
Co, and Mn) is regarded as one of the new generations of
cathode materials for Li-ion batteries due to its high energy density,
low cost, and less toxicity. However, there still exist some drawbacks
such as its high initial irreversible capacity, capacity/voltage fading,
poor rate capability, and so forth, which seriously limit its large-scale
commercial applications. In this paper, the Ta–Mo codoped Li1.2Ni0.13Co0.13Mn0.54O2 with high energy density is prepared via a coprecipitation
method, followed by a solid–state reaction. The synthetic mechanism
and technology, the effect of charge–discharge methods, the
bulk doping and the surface structure design on the structure, morphology,
and electrochemical performances of the Li1.2Ni0.13Co0.13Mn0.54O2 cathode are systematically
investigated. The results show that Ta5+ and Mo6+ mainly occupy the Li site and transition-metal site, respectively.
Both the appropriate Ta and Ta–Mo doping are conductive to
increase the Mn3+ concentration and suppress the generation
of Li/Ni mixing and the oxygen defects. The Ta–Mo codoped cathode
sample can deliver 243.2 mA h·g–1 at 1 C under
2.0–4.8 V, retaining 80% capacity retention after 240 cycles,
and decay 1.584 mV per cycle in 250 cycles. The capacity retention
can be still maintained to 80% after 410 cycles over 2.0–4.4
V, and the average voltage fading rate is 0.714 mV per cycle in 500
cycles. Compared with the pristine, the capacity and voltage fading
of Ta–Mo codoped materials are effectively suppressed, which
are mainly ascribed to the fact that the highly valence Ta5+ and Mo6+ that entered into the crystal lattice are favorable
for maintaining the charge balance, and the strong bond energies of
Ta–O and Mo–O can help to maintain the crystal structure
and relieve the corrosion from the electrolyte during the charging/discharging
process.