Micrometer-scale single crystalline particles of niobium titanium oxide enabling an Ah-level pouch cell with superior...

Wadsley-Roth phase niobium titanium oxide (TiNb₂O₇) is widely regarded as a promising anode candidate for fast-charging lithium-ion batteries due to its safe working potential and doubled capacity in comparison to the commercial fast-charging anode material (lithium titanium oxide, Li₄Ti₅O₁₂). Although good fast charge/discharge performance was shown for nanostructured TiNb₂O₇, the small size would cause the low electrode compensation density and energy density of batteries, as well as parasitic reactions. Fundamental understanding of the electrochemical lithium insertion/extraction process and the structural evolution for the micrometer-scale single crystalline TiNb₂O₇ (MSC-TiNb₂O₇) could provide insights to understand its inherent properties and possibility for fast-charging application. Here, we revealed the highly reversible structural evolution of the MSC-TiNb₂O₇ during the lithiation/delithiation processes. Interestingly, an ion-conductive lithium niobate interphase was in situ formed on the MSC-TiNb₂O₇ surface during the formation cycle, which could facilitate fast ion diffusion on the material surface and support fast electrochemical reaction kinetics. Experimentally, the MSC-TiNb₂O₇ delivered a high reversible capacity of 291.9 mA h g^-1 at 0.5C with a high initial Coulombic efficiency (>95%), and showed superb rate capability with a reasonable capacity of 55.6 mA h g^-1 under a high current density of 40C. An Ah-level pouch cell with a lithium cobalt oxide (LiCoO₂) cathode exhibited 91.5% capacity retention at 3C charging rate, which revealed the significant role of high crystallinity and in situ formation of an ion conductive nano-interphase in realizing fast charging capability of practical TiNb₂O₇-based lithium-ion batteries.