Nanocomposite Engineering of a High-Capacity Partially Ordered Cathode for Li-Ion Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 36600458.
- Also identified by DOI 10.1002/adma.202208423.
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Abstract
Understanding the local cation order in the crystal structure and its correlation with electrochemical performances has advanced the development of high-energy Mn-rich cathode materials for Li-ion batteries, notably Li- and Mn-rich layered cathodes (LMR, e.g., Li<sub>1.2</sub> Ni<sub>0.13</sub> Mn<sub>0.54</sub> Co<sub>0.13</sub> O<sub>2</sub> ) that are considered as nanocomposite layered materials with C2/m Li<sub>2</sub> MnO<sub>3</sub> -type medium-range order (MRO). Moreover, the Li-transport rate in high-capacity Mn-based disordered rock-salt (DRX) cathodes (e.g., Li<sub>1.2</sub> Mn<sub>0.4</sub> Ti<sub>0.4</sub> O<sub>2</sub> ) is found to be influenced by the short-range order of cations, underlining the importance of engineering the local cation order in designing high-energy materials. Herein, the nanocomposite is revealed, with a heterogeneous nature (like MRO found in LMR) of ultrahigh-capacity partially ordered cathodes (e.g., Li<sub>1.68</sub> Mn<sub>1.6</sub> O<sub>3.7</sub> F<sub>0.3</sub> ) made of distinct domains of spinel-, DRX- and layered-like phases, contrary to conventional single-phase DRX cathodes. This multi-scale understanding of ordering informs engineering the nanocomposite material via Ti doping, altering the intra-particle characteristics to increase the content of the rock-salt phase and heterogeneity within a particle. This strategy markedly improves the reversibility of both Mn- and O-redox processes to enhance the cycling stability of the partially ordered DRX cathodes (nearly ≈30% improvement of capacity retention). This work sheds light on the importance of nanocomposite engineering to develop ultrahigh-performance, low-cost Li-ion cathode materials.