High-Volumetric-Energy-Density Cathode Material from Single-Sized Precursor via Precise Additive Control

Abstract

To overcome the energy density limitations of current layered cathode materials, high-nickel cathode materials with a bimodal distribution composed of ∼ 15um-sized secondary particles and micron-sized single crystals are synthesized from a single-sized high-nickel precursor by incorporating the grain-growth promoting/inhibiting additive. Synthesized cathode material effectively reduces the pores within the electrode and shows an excellent electrode density of > 3.9 g/cm3, exceeding ∼ 80 % of the theoretical density. In addition, due to efficient contact between large secondary particles and small single crystals, bimodal particles with additives show higher electrical conductivity compared to additive-free monomodal secondary particles, and a capacity of ∼ 220 mAh/g is achieved even at a high loading level of ∼ 30 mg/cm2 and 96 % active-material fraction. Based on remarkable electrode density and high capacity, it is possible to realize a volumetric energy density of more than 700 mAh/cm3. To the best of our knowledge, this is the highest energy density result for electrodes made from layered cathode materials. Moreover, through the synergistic effect of morphology control by selective additives and surface coating, the synthesized bimodal cathode simultaneously exhibits excellent capacity as well as improved cycle-life performance compared to a bare cathode without additives. The enhanced electrochemical performance is attributed to increased connectivity between individual cathode particles, decreased bulk/surface resistance, and reduced intergranular cracks after cycling through structure design by additives, which is confirmed through various electrochemical analyses and electrode observations.