Abstract
Earth-abundant TiO(2) is a promising negative electrode for low-cost sodium-ion batteries (SIBs) owing to its high capacity, rapid (dis)charging capability, safe operation potential and nonflammability. Crystalline anatase TiO(2) is not suitable for reversible Na(+) (de)intercalation, but it displays pseudocapacitive response after repeated cycles. Herein, we find and demonstrate that ordered rocksalt (RS) NaTiO(2) nanograins are in situ formed by electrochemically cycling with Na(+) ions in anatase and amorphous TiO(2). The in situ formed RS-NaTiO(2) follows a solid-solution reaction with small volume changes of only 2.0%, that determines the pseudocapacitive "mirror-like" cyclic voltammetry curve with a couple of broad redox peaks at 0.75 V vs. Na(+)/Na, a high capacity of 253 mAh g(-1), high-rate capability and thousands of stable cycles. The multistep crystalline-to-amorphous-to-RS transformations are able to be electrochemically activated during the aging process of assembled full cells. Our finding provides a direction for developing unconventional Ti-based high-performance active materials for SIBs with both high energy and power densities.