The global shift towards electric vehicles and large-scale energy storage systems necessitates cost-effective and abundant alternatives to commercial Co/Ni-based cathodes, such as LiNi0.6Mn0.2Co0.2O2, for Li-ion batteries (LIBs). Manganese-based disordered rock-salts (Mn-DRXs) have shown promising potential to outperform conventional cathodes at a lower cost, achieving energy densities exceeding 900 Wh kg-AM (per active material, AM).[1-4] However, previous demonstrations of such performance have been conducted in cell constructions that are far from commercially viable, utilizing diluted electrode films (∼70 wt%-AM) containing excessive carbon and binder.[3] In this presentation, I will address the challenges associated with attaining AM-concentrated Mn-DRX cathodes (>95 wt%-AM).[5] It will be revealed that the failures observed in AM-concentrated electrodes of Mn-DRXs stem from their remarkably low electrical conductivity (ranging from 10−10 to 10−8 S/cm) and the subsequent collapse of the electrode's electrical network due to volume changes over cycling. I will then outline strategies to mitigate these challenges through electrical percolation engineering and the enhancement of electrode mechanical properties. Through these approaches, we have successfully demonstrated nearly all-AM Mn-DRX cathodes (∼96 wt%-AM) and achieved the highest application-level energy density (∼1050 Wh kg-cathode) reported to date.[5] Furthermore, I will discuss the trade-off associated with the manganese content in Mn-DRXs concerning their electrical conductivity and volume change behavior. This discussion will provide valuable insights and guidelines for material design aimed at advancing Co/Ni-free LIBs' technology readiness.Overall, this presentation will shed light on the current status, challenges, and breakthroughs in the development of Mn-DRX cathodes, offering a pathway towards more efficient and sustainable LIB technology. References J. Lee et al., Science 343, 519−522 (2014).J. Lee et al., Nature 556, 185–190 (2018).H. Li, R. Fong, D.-H. Seo, J. Lee et al., Joule 6, 53–91 (2022).E. Lee, H. Lee, J. Lee, D.-H. Seo et al., Adv. Mater. 35, 2208423 (2023).E. Lee, D.-H. Lee, D.-H. Seo, J. Lee et al., Energy Environ. Sci. (2024) https://doi.org/10.1039/D4EE00551A.
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