Synergy of a hierarchical porous morphology and anionic defects of nanosized Li4Ti5O12 toward a high-rate and large-capacity lithium-ion battery

Abstract Exploring electrode materials with a high volumetric energy density and high rate capability remains of a great challenge for nanosized-Li4Ti5O12 (LTO) batteries. Here, hierarchical porous Ti3+-C-N-Br co-doped LTO (LTOCPB-CC) is synthesized using carboxyl-grafted nanocarbon (CC) and cetylpyridinium bromide (CPB) as combined structure-directing agents. Ti4+-O-CPB/Li+-CC is designed as a new molecular chelate, in which CPB and CC promote the uniform mixing of Li+ and Ti4+ and control the morphology of TiO2 and the final product. The defects (oxygen vacancies and ion dopants) formed during the annealing process increase the electron/hole concentration and reduce the band gap, both of which enhance the n-type electron modification of LTO. As-prepared LTOCPB-CC has a large specific surface area and high tap density, as well as a high electronic conductivity (2.84 × 10−4 S cm−1) and ionic conductivity (3.82 × 10−12 cm2 s−1), which are responsible for its excellent rate capability (157.7 mAh g−1 at 20 C) and stable long-term cycling performance (0.008 % fade per cycle after 1000 cycles at 20 C).