Size‐Independent Fast Ion Intercalation in Two‐Dimensional Titania Nanosheets for Alkali‐Metal‐Ion Batteries

Compared to lithium ions, the fast redox intercalation of large-radius sodium or potassium ions into a solid lattice in non-aqueous electrolytes is an elusive goal. Herein, by regulating the interlayer structure of stacked titania sheets through weakened layer-to-layer interactions and a robustly pillared gallery space, the two-dimensional channel between neighboring sheets was completely open to guest intercalation, allowing fast intercalation that was practically irrespective of the carrier-ion sizes. Regardless of employing regular Li or large-radius Na and K ions, the material manifested zero strain-like behavior with no significant change in both host structure and interlayer space, enabling comparable capacities for all tested ions along with excellent rate behaviors and extraordinarily long lifetimes, even with 80-μm-thick electrodes. The result highlights the importance of interlayer structural features for unlocking the electrochemical activity of a layered material.