Suppressing gas swelling in self-assembled Li4Ti5O12 (400) for high-performance rechargeable batteries

Lithium titanate is a promising anode material for lithium-ion batteries due to its high-rate capability and long-cycle duration. However, gas swelling during electrochemical reactions has hindered its industrial application. Here, we synthesize self-assembled (4 0 0)-orientation lithium titanate (SA-LTONF) with ultrafine nanoparticles using a feasible thermal method. The SA-LTONF with an organic carbon coating exhibited superior electro-chemical performance. To understand such high-rate capability, we perform density functional theory (DFT) calculations which elucidate the orientation-dependent electrochemical mechanism of hydrogen evolution and the atomically dynamic mechanism of lithium-ion migration in Li4Ti5O12 and Li7Ti5O12. Our findings provide a unique insight into the gas generation and ultrafast lithium-ion transportation in lithium titanate and offer guidance for nanoarchitecture construction and materials design of lithium titanate for commercial applications.