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

Freestanding film electrode comprising face-to-face alternately stacked 2D TiO2 nanosheets and reduced graphene oxide (rGO) is designed and fabricated as binder-free anode for lithium-ion batteries. The ultrathin TiO2 nanosheets with (001) facet exposed having the lowest Li+ diffusion barrier face-to-face hetero-assembled onto the conductive rGO, the Li+ can swiftly diffuse into the TiO2 nanosheets across the (001) facets with the lowest barrier and short transfer distance. The spectacular configuration of this planary-aligned electrode leads to superior performances than other composite electrodes previously reported, which delivers a large capacity of 132.3 mA h g-1 with capacity retention of 89 % over 1,000 cycles at a high rate of 20 C (1 C = 168 mA g-1). This work proved that controlling the arrangement orientation of electrode materials with anisotropy Li+ diffusion barrier could remarkably improve the electrochemical properties, boosting promising application in high-power energy storage devices.