Freestanding Nanoengineered [001] Preferentially Oriented TiO₂ Nanosheets−Graphene Planarly Aligned Nanohybrids with Enhanced Li‐Storage Properties

Abstract A freestanding film electrode comprising face‐to‐face alternately stacked 2D TiO 2 nanosheets and reduced graphene oxide (rGO) is designed and fabricated as a binder‐free anode for lithium‐ion batteries. The ultrathin TiO 2 nanosheets, with (001) facets exposed were face‐to‐face hetero‐assembled onto the conductive rGO, allowing Li + to swiftly diffuse into the TiO 2 nanosheets across the (001) facets with the lowest barrier and a short transfer distance. The configuration of this planar‐aligned electrode leads to superior lithium performance, which delivers a large capacity of 132.3 mA h g −1 with a capacity retention of 89 % over 1000 cycles at a high rate of 20 C (1 C=168 mA g −1 ). This work proves that controlling the arrangement orientation of electrode materials with an anisotropy Li + diffusion barrier could remarkably improve the electrochemical properties, for promising applications in high‐power energy‐storage devices.