Na-ion cathode materials cycling at high voltages with long cycling life and high capacity are of imminent need for developing future high-energy Na-ion batteries. However, the irreversible anionic redox activity of Na-ion layered cathode materials results in structural distortion and poor capacity retention upon cycling. Herein, we develop a facile doping strategy by incorporating copper into the layered cathode material lattice to relieve the irreversible oxygen oxidation at high voltages. On the basis of a comprehensive comparison with the Cu-free material, both the overoxidation of O 2− to trapped molecular O 2 and Mn-related Jahn−Teller distortion have been effectively inhibited by restraining both the oxygen activity and participation of Mn 4+ /Mn 3+ redox activity. Not limited to discovering stable cycling behavior at high voltages after Cu substitution, our findings also highlight an effective strategy to stabilize the anionic redox activity and elucidate the stabilization mechanism of Cu substitution, thus paving the way for further improvement of layered oxide cathode materials for high-energy Na-ion batteries.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.