Tailoring Electronic Structure to Achieve Maximum Utilization of Transition Metal Redox for High-Entropy Na Layered Oxide Cathodes

Charge compensation from cationic and anionic redox couples accompanying Na+ (de)intercalation in layered oxide cathodes contributes to high specific capacity. However, the engagement level of different redox couples remains unclear and their relationship with Na+ content is less studied. Here we discover that it is possible to take full advantage of the high-voltage transition metal (TM) redox reaction through low-valence cation substitution to tailor the electronic structure, which involves an increased ratio of Na+ content to available charge transfer number of TMs. Taking NaxCu0.11Ni0.11Fe0.3Mn0.48O2 as the example, the Li+ substitution increases the ratio to facilitate the high-voltage TM redox activity,…

• NN
  National Natural Science Foundation of China

  Awards: 52202332, 52122214, 52072403
• CP
  China Postdoctoral Science Foundation

  Award: 2021M703460
• YI
  Youth Innovation Promotion Association of the Chinese Academy of Sciences

  Award: 2020006
• NK
  National Key Research and Development Program of China

  Award: 2022YFB2402500