Abstract

With the rising cost and insufficient supply of cobalt, the thrust for cobalt-free cathode materials with the high specific capacity to build Li-ion batteries has increased significantly. Using nickel as the prime electrochemical active species, we have synthesized a new-class of materials with the combination of ordered and disordered phases. To obtain high capacity and electrical charge neutrality, stoichiometry of cations designed in a way that it forms Li/Ni rich Ni-Ti-Mo oxide materials. In addition to conventional capacity from redox activity of transition metals, partially reversible oxygen redox reaction also contributes to electrochemical activity and thus results in unusual high capacity. The resultant cathode materials of LiNi0.5Ti0.5O2-(Li4MoO5)0.8 and LiNiO2 mixture phases reach the specific capacity of 240 mAh/g. Detailed soft X-ray absorption spectroscopy and electron microscopy are used to reveal the crystal phases in this system and trace changes in the Ni2+/Ni4+ redox couple during charge-discharge processes. Such comprehensive analysis of ordered-disordered oxides suggesting potentiality to develop high-capacity cobalt-free cathodes.

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