One-Step Synthesis of a Nanosized Cubic Li₂TiO₃-Coated Br, C, and N Co-Doped Li₄Ti₅O₁₂ Anode Material for Stable High-Rate Lithium-Ion Batteries

Nanosized Li4Ti5O12 with both a Li2TiO3 coating and C–N–Br co-doping (CLLTO) was successfully synthesized via a facile reverse microemulsion method in one step using hexadecyl trimethyl ammonium bromide as a surface control agent and as a carbon, nitrogen, and bromine source. A uniform Li2TiO3 layer was formed on the surface and strongly adhered to the host material Li4Ti5O12 (LTO), which played an important role in improving the cyclic stability of CLLTO. The thin and stable Li2TiO3 layer has the same cubic structure as LTO, which provides many three-dimensional channels for ion transport. C, N, and Br co-doping in CLLTO promoted the transition of Ti4+ to Ti3+ in Li4Ti5O12, which could improve the capacity and facilitate the Li+ ion and electron transfer at the interface. The conductive behavior induced by co-doping was estimated by UV–vis diffuse reflectance spectra and further supported by theoretical calculations. The electrical conductivity of both p-type and n-type LTO can be well improved by co-doping C, N, and Br. This improvement may be due to the band gap reduction and the increased n-type electronic modification of the entire LTO. Owing to the synergistic effect of coating, co-doping, and nanosizing at one time, the CLLTO exhibits a high discharge capacity of 177.3–153.9 mA h g–1 at the working rate of 0.1C–20C, with a capacity retention of 86%. The stable cycling of CLLTO is also obtained after 500 cycles at 20C, with a capacity retention of 95.5% (approximately 8 times higher than that of pure LTO) and almost 100% Coulombic efficiency. With high capacity, excellent rate performance, and good cycling stability, CLLTO can be applied in high-power lithium-ion batteries.