Modulating Grain Boundary Networks to Achieve Superior Chemomechanical Coupling Properties in Nickel-Rich Cathode Materials.

To forge ahead with the next generation of power batteries boasting superior energy density, nickel-rich layered oxides are regarded as some of the most promising cathode materials. However, challenges such as microcracks, which are attributed to the elevated nickel content of the materials, have posed impediments to their further development and application. Consequently, this article focuses on the understanding of the materials in the deep delithiation state, dissecting their degradation mechanisms through a dual lens of electrochemical and mechanical properties. The comprehensive analysis reveals that microcracks within the particles exhibit a degree of reversibility. However, with repeated Li de-/intercalation, these microcracks progressively propagate and permeate the entire particle, ultimately leading to particle fragmentation. Therefore, this study employs DyO as an inducer to facilitate the growth of primary crystal grains, reducing the internal porosity of the particles. This effectively enhances the conductivity and lithium-ion diffusion kinetics in deep lithium-ion deintercalation states of nickel-rich cathode materials. The modified material exhibits significant suppression of microcrack formation and growth during cycling, leading to notable improvements in its chemical-mechanical properties. These degradation mechanisms and modification strategies of Ni-rich cathodes offer valuable insights into the development of Ni-rich cathode materials tailored for electric vehicles.