A combination
of the solution combustion and mechanochemical syntheses
(SC-MS) presents a facile, low-energy, and cost-effective method to
prepare layered lithium-rich oxide (LLO) composites and core-shell
structures compared to the conventional methods of preparing these
compounds. The composite and core-shell structures of xLi2MnO3·(1 – x)LiNi0.5Mn0.3Co0.2O2 (0 ≤ x ≤ 0.7) were prepared using optimized SC-MS and
were comparatively characterized with respect to their morphology,
chemical composition, and structural and electrochemical properties.
Notably, the composite cathode materials show lower discharge capacities
compared to the core-shell cathode materials with same target stoichiometry
but comparable cycling stability, which was ascribed to their probably
higher contents of Ni3+. Apart from giving larger unit
cell volumes, the core-shell cathode materials with a Ni-rich core
and a Mn-rich shell gave a combination of higher discharge capacity,
good cyclability, lower irreversible capacity loss, better rate performance,
and thermal stability. This confirms the efficiency of the core-shell
strategy in improving the electrochemical performance of LLOs, especially
for systems with a Ni-rich component. These results show that the
SC-MS method could be used for the large-scale synthesis of electrode
materials for high power Li-ion batteries.