Abstract
The complete solid solutions in the pseudo-binary LiNi 1/3Co 1/3Mn 1/3O 2–LiMg 1/3Co 1/3Mn 1/3O 2 system with α-NaFeO 2 type layered rock-salt structure have been successfully synthesized. The replacement of Ni with Mg atoms has enhanced the diffraction intensity due to cation ordering in α-NaFeO 2 type structure. Powder X-ray diffraction (XRD) patterns of LiMg 1/3Co 1/3Mn 1/3O 2 show a broad and diffuse peak with an intensity maximum at around d = 4.2 Å indicating an in-plane [√3 × √3] R30° type ordering. Electron diffraction (ED) patterns also show clear and intense superlattice spots due to the in-plane [√3 × √3] R30° type ordered layers. However, the [√3 × √3] R30° type ordered layers are almost randomly stacked as evidenced by diffuse scattering in the powder XRD and ED patterns. The TEM lattice image clearly reveals the random stacking. XRD and ED patterns agree with the simulated ones using the DIFFaX program based on the above structural model. Solid solution LiNi 1/3− x Mg x Co 1/3Mn 1/3O 2 (0.0 ≤ x ≤ 0.33) also show a similar two dimensional cation ordering. Electrochemical measurements of LiNi 1/3− x Mg x Co 1/3Mn 1/3O 2 indicate that not only Ni but also Co can be active as redox species in this solution system. The redox potential of Co in LiMg 1/3Co 1/3Mn 1/3O 2 is about 4.1 V.
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