Synthesis and electrochemical properties of layer-structured 0.5Li(Ni0.5Mn0.5)O2–0.5Li(Li1/3Mn2/3)O2 solid mixture

A 1:1 mixture of electrochemically active Li(Ni0.5Mn0.5)O2 and electrochemically inactive Li(Li1/3Mn2/3)O2, i.e. Li(Li0.17Ni0.25Mn0.58)O2, has been synthesized by a sol–gel method. The mixture was calcined at 900 °C in air for 24 h and cooled at three different rates: quenched into liquid nitrogen, 2 °C/min, and 0.5 °C/min. It was found that the crystallographic structure and electrochemical properties of Li(Li0.17Ni0.25Mn0.58)O2 highly depend on the cooling rate. The sample quenched into liquid nitrogen exhibited a long irreversible plateau at ca. 4.5 V during the first charge, and the discharge capacity gradually increased from 170 to 210 mAh/g after 40 cycles. The samples cooled at slower rates exhibited more monoclinic character and cubic spinel phase was observed; they showed no plateaus at 4.5 V during the first charge and the discharge capacities also gradually increased from 80 and 55 mAh/g to 130 and 85 mAh/g for 2 and 0.5 °C/min-cooled samples, respectively.