Morphology Reshaping Enabling Self-Densification of Manganese Oxide Hybrid Materials for High-Density Lithium Storage Anodes

Morphology reshaping or reconfiguration, a concept widely used in plastic surgery, energy harvesting, and reconfigurable robots, is introduced for the first time to construct densified electrodes and realize compact Li-ion storage desirable for high specific energy storage field. Hausmannite-based hybrid materials, as a proof-of-concept prototype, engineered by 1-methyl-2-pyrrolidinone-soluble surface/interface organic encapsulation, which is crucial in reshaping, exhibit a remarkable increase in the volumetric capacity of more than five times after this process (approximate to 1889 Ah L-1 vs approximate to 322 Ah L-1). With the simultaneous maintenance of the intrinsic nature, good contact, and no collapsed/agglomerated unit structures of the materials in electrodes, the design affords a maximal increase in the packing compactness and manifests no sacrifice of the reversible ion storage capability (1150 mAh g(-1) at 40 mA g(-1)), stable cycling (approximate to 100% capacity retention), high rate performance (185 mAh g(-1) at 10 A g(-1)), and long lifespan (1000 cycles with 108% capacity retention, approximate to 455 mAh g(-1) at 3 A g(-1)) for relatively highly loaded electrodes (active materials: 1.20-5.34 mg cm(-2)). The concept may not only shed new light on fabricating advanced Si-based and other high capacity-related densified Li storage electrodes but also inject fresh vitality into the field of high-density power sources.