The global transition to electric vehicles and large-scale energy storage systems requires cost-effective and abundant alternatives to commercial Co/Ni-based cathodes (e.g., LiNi_0.6Mn_0.2Co_0.2O₂) for Li-ion batteries (LIBs). Manganese-based disordered rock-salts (Mn-DRXs) can outperform conventional cathodes at lower cost, achieving >900 W h kg_-AM⁻¹ (per active material, AM), but such performance has been demonstrated exclusively in cell constructions far removed from commercial viability, namely with diluted electrode films (∼70 wt%_-AM) containing excessive carbon and binder. Herein, our work involves a comprehensive study to attain AM-concentrated Mn-DRX cathodes (>95 wt%_-AM), covering from inherent material properties to the microstructure of electrodes, to address the formidable challenges in Mn-DRX research. We reveal that Mn-DRXs’ failures in AM-concentrated electrodes originate from their extremely low electrical conductivity (10⁻¹⁰–10⁻⁸ S cm⁻¹) and the collapse of the electrical network with volume change over cycling. These failure modes are resolved through electrical percolation engineering and enhancement of electrode mechanical properties, allowing our demonstration of nearly all-AM Mn-DRX cathodes (∼96 wt%_-AM) and the highest application-level energy density (∼1050 W h kg_-cathode⁻¹) reported to date. This work further unveils the trade-off role of Mn-content on Mn-DRXs’ electrical conductivity and volume change, providing guidelines for material design to advance Co/Ni-free LIBs’ technology readiness.

中文翻译：

---

用于锂离子电池的几乎全活性材料阴极，不含镍和钴

全球向电动汽车和大规模储能系统的过渡需要具有成本效益且丰富的锂离子电池（LIB）商用Co/Ni基阴极（例如LiNi _0.6 Mn _0.2 Co _0.2 O ₂ ）替代品。锰基无序岩盐 (Mn-DRX) 可以以更低的成本超越传统阴极，实现 >900 W h kg _-AM ^-1（每种活性材料，AM），但这种性能仅在远远超出的电池结构中得到证明从商业可行性来看，即使用含有过量碳和粘合剂的稀释电极膜（~70 wt% _-AM ）。在此，我们的工作涉及全面研究以获得 AM 浓缩的 Mn-DRX 阴极（> 95 wt% _-AM），涵盖从固有材料特性到电极的微观结构，以解决 Mn-DRX 研究中的艰巨挑战。我们发现，Mn-DRX 在 AM 浓缩电极中的失效源于其极低的电导率 (10 ^-10 –10 ^-8 S cm ^-1 ) 以及循环过程中体积变化导致的电网崩溃。这些失效模式通过电渗透工程和电极机械性能的增强得到解决，使我们能够演示几乎全AM Mn-DRX阴极（∼96 wt% _-AM）和最高应用级能量密度（∼1050 W h kg）_-阴极^-1）迄今为止报告。这项工作进一步揭示了锰含量对 Mn-DRX 电导率和体积变化的权衡作用，为材料设计提供指导，以推进无钴/镍锂离子电池的技术准备。