High‐Pressure Induction and Quantitative Regulation of Oxygen Vacancy Defects in Lithium Titanate

Abstract Inspired by the functional properties of ion defect induction and charge compensation in defect engineering, these methods are expected to be an effective strategy to solve the constraints of Li₄Ti₅O₁₂ (LTO) inherent conductivity and diffusion dynamics, and further improve battery rate performance. The oxygen vacancy (OV) content in LTO can be controlled quantitatively by high‐pressure induction using the high‐pressure and high‐temperature (HPHT) method. In addition, the relationship between the electrochemical properties and OV is further explored. The theoretical calculations indicate that the OV defects cause the electrons to delocalize into the conduction band of the LTO, and thus fundamentally improve the intrinsic conductivity. In particular, the high‐pressure quenching strategy of HPHT causes LTO to instantly produce crack holes with massive crystalline layers, which can be regarded as storage for the electrolyte to facilitate ion diffusion. The fabricated LTO anodes containing OVs compensate for the limitation of the poor rate performance with a capacity of 176 mAh g⁻¹ at 20 C. Pressure‐induced OV defects not only open up a new perspective in the field of lithium‐ion batteries (LIBs), but also provide a certain degree of freedom for the functional design characteristics of defect engineering.