Solid-state self-template synthesis of Ta-doped Li₂ZnTi₃O₈ spheres for efficient and durable lithium storage

Ta-doped Li₂ZnTi₃O₈ (LZTO) spheres (Li₂ZnTi_3- Ta O₈; where x is the synthetic chemical input, x = 0, 0.03, 0.05, 0.07) are synthesized via solid-state reaction using mesoporous TiO₂ spheres as the self-template. The majority of Ta⁵⁺ ions are uniformly doped into crystal lattices of LZTO through the Ti↔Ta substitution, and the rest forms the piezoelectric LiTaO₃ secondary phase on the surface, as confirmed by X-ray diffraction refinement, Raman spectroscopy, density functional theory, and electron microscopy. Electrochemical impedance spectroscopy demonstrates that the Ta⁵⁺ doping creates rapid electronic transportation channels for high Li⁺ ion diffusion kinetics; however, the LiTaO₃ surface coating is beneficial to improve the electronic conductivity. At the optimal x = 0.05, Li₂ZnTi_3- Ta O₈ spheres exhibit a reversible capacity of 90.2 mAh/g after 2000 cycles with a high coulombic efficiency of ≈100% at 5.0 A/g, thus enabling a promising anode material for lithium-ion batteries with high power and energy densities.