Determining
the impact of precursor properties is essential for
the performance regulation of LiFePO4 cathode material
prepared by carbothermic reduction. In this study, FePO4 with different crystallinities, as precursors, was obtained at various
precalcinating temperatures and reduced to form LiFePO4/C to quantitatively investigate crystallinity’s influence.
The characterization and molecular dynamics (MD) simulation results
showed that the crystallinity of FePO4 increased markedly
with a higher dehydration temperature, while excessive sintering would
occur at 700 °C, resulting in a severe particle aggregation.
The electrochemical analysis manifested that FePO4 crystallinity
would not affect the cyclic stability of cathode materials, but a
moderate dehydration temperature of the precursor could equip LiFePO4/C with the best performance via an excellent balance between
crystallinity and charge transfer. The excessive sintering and low
crystallinity both brought about obvious reduction to the discharge
capacity of LiFePO4/C such that the discharge capacity
at a 0.1 C rate would decrease from the optimum of 151.8 mAh·g–1 to less than 121.0 mAh·g–1 and 141.0 mAh·g–1 for the precursors calcinated
at 500 and 700 °C, respectively. Our work provides a clear understanding
of the non-negligible role of FePO4 crystallinity and a
valid direction for the control of the electrochemical performances
of LiFePO4.