Abstract
Lithium diffusion properties of LiMn1-xFexPO4 synthesized by hydrothermal methods were characterized from electrochemical and structural analysis. Structural defects such as cation mixing in LiMn1-xFexPO4 impede the lithium-ion diffusion. Therefore, it is important to understand effects of cation mixing in LiMn1-xFexPO4 on lithium diffusivity of LiMn1-xFexPO4. The amount of cation mixing of lithium and Mn/Fe in LiMn1-xFexPO4 was obtained by means of neutron diffraction measurements. Rietveld refinements indicated that cation mixing in the prepared LiMn1-xFexPO4 was negligible. Apparent chemical diffusion coefficients (Dapp) of lithium of LiMn1-xFexPO4 dependent on the Mn/Fe ratio were obtained by potential-step chronoamperometry (PSCA) measurements of thin composite electrodes. Dapp of lithium insertion or extraction reaction of LiMn1-xFexPO4 for Mn2+/Mn3+ increased with Fe content. Dapp for Fe2+/Fe3+ slightly increased with decreasing Fe content. The difference of Dapp value was attributed to the activation energies (Ea) of lithium diffusion process of LiMn1-xFexPO4. The Ea of LiMn1-xFexPO4 for Mn2+/Mn3+ and Fe2+/Fe3+ was determined by the energy barrier of lithium hopping at the interphase between Li-rich and Li-poor phase under electrochemical kinetic conditions.
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