Descriptor-informed multi-component doping enables high-performance Co-free Ni-rich cathodes

Abstract

Co-free Ni-rich layered oxide cathodes hold great promise for cost-effective, high-energy lithium-ion batteries, but their practical application remains limited by sluggish Li+ kinetics and rapid capacity fading. Although doping has been widely used to mitigate these issues, conventional trial-and-error dopant selection remains inefficient for guiding rational materials development. Here we move beyond empirical dopant screening by developing a descriptor-informed multi-component dopant selection strategy based on dopant charge density and metal–oxygen bond strength. Low-charge-density dopants reduce electrostatic barriers to Li+ migration, while high-bond-energy dopants reinforce the oxygen sublattice and stabilize the metal–oxygen framework. This doping strategy simultaneously accelerates Li+ kinetics, suppresses cycling-induced phase transitions and mitigates chemomechanical fatigue, thereby delivering exceptional electrochemical performance in Co-free Ni-rich cathodes. The enhanced apparent Li+ transport and structural stability enable an ultrahigh-rate capability of 130.9 mAh g−1 at 25 C and at 25 °C, excellent cycling retention of 82.4% after 350 cycles at 10 C and robust low-temperature operation delivering 112.2 mAh g−1 at 1 C under −20 °C. These findings, transitioning the design principle from empirical or trial-based selection to a targeted selection regime, present a promising route for developing high-performance cathode materials for lithium-ion batteries.