Ni-rich
Li(Ni1–x–y
Co
x
Mn
y
)O2-based cathodes still suffer from low cycling stability,
which arises from capacity fading and impedance rise due to parasitic
side reactions at the interface. Surface coatings have shown promising
results in stabilizing the cathode surface and improving the cycling
stability. However, a comprehensive understanding on the beneficial
effect of the coating is still missing. In this paper, we used a solution-based
technique to coat Ni-rich Li(Ni0.70Co0.15Mn0.15)O2 with a thin Al2O3 layer
followed by post-annealing at 600 °C. Electrochemical characterization
shows a drastic improvement of the cathode’s cycling stability
due to the coating. After post-annealing, the cycling stability is
even further improved, accompanied with its C-rate performance. Structural
characterization confirms that annealing results in the formation
of an amorphous Al2O3/LiAlO2 coating
layer, which exhibits increased lithium-ion conductivity compared
to the Al2O3 coating. More importantly, temperature-dependent
impedance measurements reveal that the coatings do not affect the
activation energy of the charge transport, which guarantees a sufficient
electronic conductivity between the secondary NCM particles in the
cathode. Thus, the Al2O3/LiAlO2 layer
not only inhibits direct contact between electrode and electrolyte,
preventing side reactions and stabilizes the performance, but also
facilitates conductive pathways for lithium ions while preserving
the electronic connectivity between cathode’s particles, leading
to a low interfacial resistance and excellent rate capability. The
results show the importance of providing a sufficiently high electrical
conductivity accompanied with low activation energies in coating layers
for both ions and electrons, which needs to be considered in design
strategies for next-generation lithium-ion batteries.