High performance LiFePO4 nanomaterial obtained by a tavorite-to-olivine phase transition at low-temperature

The paper reports the preparation of nanostructured LiFePO4 cathode with high performance by a phase transition process from the tavorite LiFePO4OH structure to the olivine LiFePO4 structure at low-temperature. On the premise of the lattice maturity, a lower crystallization temperature is conducive to synthesizing LiFePO4 with optimal unit cell, crystalline size, and electrochemical property, as well as reducing energy consumption of production. [Display omitted] •High performance LiFePO4 was obtained by a novel LiFePO4OH precursor at 550–600 °C.•The desirable LiFePO4OH precursor was prepared via a wet pre-lithiation process.•The mechanisms affecting the electrochemical performance of LiFePO4 have been studied. The main problem currently faced in the large-scale production of LiFePO4 by solid-phase methods is the high energy consumption caused by solid/melt-phase lithiation process. Herein, LiFePO4 nanoparticles are successfully obtained by a phase transition from the tavorite LiFePO4OH structure to the olivine LiFePO4 structure at low-temperature (550–600 °C). This desirable LiFePO4OH precursor is prepared via a wet pre-lithiation process, and its thermodynamic feasibility is demonstrated by thermodynamic calculation. The liquid-phase lithiation followed by a simple carbothermal reduction process (c.f., the solid/melt-phase lithiation process of the traditional solid-state method) results in a superior mass transfer efficiency and reaction uniformity. It therefore prevents the requirement for a higher temperature and longer sintering process. It is also indicated that on the premise of the lattice perfection, a lower crystallization temperature is not only conducive to widening the effective ion diffusion channels of LFP, inhibiting further crystal growth, and shortening the diffusion path, but it also reduces the synthetic cost. As a result, a crystallization temperature of 600 °C (or 550 °C) is optimal, and the resulting LiFePO4 electrode can deliver an appealing high rate capacity of 147.7 mA h g−1 at 10 C. It is expected that this novel synthetic route could be employed for the large-scale commercial production of high performance LiFePO4 cathode materials at a low cost.