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

摘要

Abstract 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 (≈1889 Ah L −1 vs ≈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 (≈100% capacity retention), high rate performance (185 mAh g −1 at 10 A g −1 ), and long lifespan (1000 cycles with 108% capacity retention, ≈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.