Structural Design Principle of Rocksalt Oxides for Li-Excess Cathode Materials.
basic_science · Level V
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- Record sourced from PubMed, PMID 38207327.
- Also identified by DOI 10.1021/acsnano.3c10193.
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Abstract
Li-excess oxide cathodes have received increasing attention due to their high capacity derived from accumulated cation and anion redox activity. However, Li-excess layered oxides suffer from capacity and voltage decay due to the irreversible phase transition, while cation-disordered cathodes also have the problems of poor cycling stability and rate capability. The rocksalt oxides with a layered-disordered coexistence nanostructure can combine the advantages of both phases such as the inherent high capacity of Li-excess oxides, good rate capability of the layered phase, and structural stability resulting from the intergrown disordered phase. Herein, for rational design, we developed a descriptor by correlating the ionic radius and electronic configuration to predict layered, cation-disordered, and coexistent structures of Li-excess cathode materials. Accordingly, we experimentally synthesized Li<sub>1.2</sub>Ni<sub>0.4</sub>Mn<sub>0.2</sub>Nb<sub>0.2</sub>O<sub>2</sub> oxide with a coexistent structure in which the layered and disordered phases are well combined in the nanoscale region, achieving a high capacity (312 mAh g<sup>-1</sup>) with good cycling stability and rate capability. The design principle with composition predicting structure provides a valuable strategy in controllably designing and preparing Li-excess cathode materials.