Self‐Supporting and Binder‐Free Anode Film Composed of Beaded Stream‐Like Li₄Ti₅O₁₂ Nanoparticles for High‐Performance Lithium‐Ion Batteries

Abstract A self‐supporting film composed of arrays of Li 4 Ti 5 O 12 (LTO) nanoparticles (NPs) prepared through chemical lithiation of anodic TiO 2 nanotube arrays and calcination in air is used as a high‐performance binder‐free anode in lithium‐ion batteries (LIBs). The LTO nanoparticles formed in situ are closely connected along the axial direction of the pristine TiO 2 nanotubes, forming a beaded stream‐like structure. The self‐supporting NPs film has a large tap density and overall packing factor, and the three‐dimensional (3D) network of NPs increases the electroactive interface, facilitating transfer of Li + and enhancing the intercalation kinetics during charging/discharging. The LTO electrode with excellent mechanical flexibility and robustness has a volumetric capacity of 304 mAh cm −3 at a current density of 50 mA cm −3 as well as a high rate capability of 208 mAh cm −3 at 5000 mA cm −3 . After undergoing 500 cycles at a high current density of 1250 mA cm −3 , 91.4 % of the capacity is retained, demonstrating high reversibility and cycling stability of the binder‐free LTO NPs film electrode in LIBs.