Cycling-Induced Capacity Increase of Bulk and Artificially Layered LiTaO₃ Anodes in Lithium-Ion Batteries

Tantalum-based oxide electrodes have recently drawn much attention as promising anode materials owing to their hybrid Li⁺ storage mechanism. However, the utilization of LiTaO₃ electrode materials that can deliver a high theoretical capacity of 568 mAh g^-1 has been neglected. Herein, we prepare a layered LiTaO₃ electrode formed artificially by restacking LiTaO₃ nanosheets using a facile synthesis method and investigate the Li⁺ storage performance of this electrode compared with its bulk counterpart. The designed artificially layered anode reaches specific capacities of 474, 290, and 201 mAh g^-1, respectively, at 56 (>500 cycles), 280 (>1000 cycles), and 1120 mAg^-1 (>2000 cycles) current densities. We also determine that the Li⁺ storage capacity of the layered LiTaO₃ demonstrates a cycling-induced capacity increase after a certain number of cycles. Adopting various characterization techniques on LiTaO₃ electrodes before and after electrochemical cycling, we attribute the origin of the cycling-induced improvement of the Li⁺ storage capacity in these electrodes to the amorphization of the electrode after cycling, formation of metallic tantalum during the partially irreversible conversion mechanism, lower activation overpotential of electrodes due to the formation of Li-rich species by the lithium insertion mechanism, and finally the intrinsic piezoelectric behavior of LiTaO₃ that can regulate Li⁺ diffusion kinetics.