Hexagonal MoO3 Anode with Extremely High Capacity and Cyclability for Lithium-Ion Battery: A Combined Theoretical and Experimental Study

It is essential and still remains a big challenge to obtain fast-charge anodes with large capacities and long lifespans for Li-ion batteries (LIBs). Among all of the alternative materials, molybdenum trioxide shows the advantages of large theoretical specific capacity, distinct tunnel framework, and low cost. However, there are also some key shortcomings, such as fast capacity decaying due to structural instability during Li insertion and poor rate performance due to low intrinsic electron conductivity and ion diffusion capability, dying to be overcome. A unique strategy is proposed to prepare Ti-h-MoO3–x @TiO2 nanosheets by a one-step hydrothermal approach with NiTi alloy as a control reagent. The density functional theory (DFT) calculations indicate that the doping of Ti element can make the hexagonal h-MoO3–x material show the best electronic structure and it is favor to be synthesized. Furthermore, the hexagonal Ti-h-MoO3–x material has better lithium storage capacity and lithium diffusion capacity than the orthogonal α-MoO3 material, and its theoretical capacity is more than 50% higher than that of the orthogonal α-MoO3 material. Additionally, it is found that Ti-h-MoO3–x @TiO2 as an anode displays extremely high reversible discharge/charge capacities of 1326.8/1321.3 mAh g–1 at 1 A g–1 for 800 cycles and 611.2/606.6 mAh g–1 at 5 A g–1 for 2000 cycles. Thus, Ti-h-MoO3‑x @TiO2 can be considered a high-power-density and high-energy-density anode material with excellent stability for LIBs.