The Ni/Li disordering evolution mechanisms in Ni-based layered cathode materials: insights from first-principles calculations

The origin of Ni/Li disordering in Ni-based layered cathode materials is investigated using first-principles calculations. The correlation between interlayer distance, Li vacancies, valence state, ionic radius, coordination polyhedron size, and Ni/Li disordering is determined. Existing Ni/Li disordering accelerates further degradation of such disordering. The synergistic migration of Li and Ni significantly reduces migration energy, which is proposed as the key evolution mechanism driving Ni/Li disordering during synthesis and charge–discharge cycles.