Lithium-rich layered oxides are promising cathode materials for high-energy-density lithium-ion batteries. However, the development of cathode materials based on these layered oxides has been limited by voltage fading, poor rate performance, and the low tap density of these materials. In this work, we prepared a material consisting of micrometer-scale spherical lithium-rich layered oxide particles with a three-dimensional conductivity network design and modified the surface of the primary particles with ruthenium. The as-obtained product with a maximum tap density of 2.1 g cm-3 shows a superior high reversible capacity with 280 mA h·g-1 at 0.1 C, a capacity retention of 98.1% after 100 cycles, and an outstanding rate capability. More importantly, enrichment of the primary particle surface with ruthenium can effectively suppress voltage decay. This cathode is feasible to construct high-energy and high-power lithium-ion batteries. This novel design may furthermore open the door to new material engineering applications for high-performance cathode materials.
Keywords: DFT calculations; high-energy-density lithium-ion batteries; lithium-rich layered oxides; ruthenium segregation; suppressing voltage decay.