Synthesis of Three-Dimensional Nanoporous Li-Rich Layered Cathode Oxides for High Volumetric and Power Energy Density Lithium-Ion Batteries

As rechargeable Li-ion batteries have expanded their applications into on-board energy storage for electric vehicles, the energy and power must be increased to meet the new demands. Li-rich layered oxides are one of the most promising candidate materials; however, it is very difficult to make them compatible with high volumetric energy density and power density. Here, we develop an innovative approach to synthesize three-dimensional (3D) nanoporous Li-rich layered oxides Li[Li_0.144Ni_0.136Co_0.136Mn_0.544]O₂, directly occurring at deep chemical delithiation with carbon dioxide. It is found that the as-prepared material presents a micrometer-sized spherical structure that is typically composed of interconnected nanosized subunits with narrow distributed pores at 3.6 nm. As a result, this unique 3D micro-/nanostructure not only has a high tap density over 2.20 g cm^-3 but also exhibits excellent rate capability (197.6 mA h g^-1 at 1250 mA g^-1) as an electrode. The excellent electrochemical performance is ascribed to the unique nanoporous micro-nanostructures, which facilitates the Li⁺ diffusion and enhances the structural stability of the Li-rich layered cathode materials. Our work offers a comprehensive designing strategy to construct 3D nanoporous Li-rich layered oxides for both high volumetric energy density and power density in Li-ion batteries.