Exploring a Co-Free, Li-Rich Layered Oxide with Low Content of Nickel as a Positive Electrode for Li-Ion Battery

The development of cathode materials represents the key bottleneck to further push the performance of current Li-ion batteries (LIB) beyond the commercial benchmark. Li-rich transition-metal-layered oxides (LRLOs) are a promising class of materials to use as high-capacity/high-potential positive electrodes in LIBs thanks to the large lithium content (e.g., similar to 1.2 Li equiv per formula unit) and the exploitation of multiple redox couples (e.g., Mn4+/3+, Co4+/3+, Ni4+/3+/2+). In this work, we propose and demonstrate experimentally a Co-free overlithiated LRLO material with a limited nickel content, i.e., Li1.25Mn0.625Ni0.125O2. This LRLO is able to exchange reversibly an outstanding practical specific capacity at room temperature, i.e., 230 mAh g(-1) at C/10 for almost 200 cycles, and can sustain high current rates, i.e., 118 mAh g(-1) at 2C. This material has been successfully prepared by a facile solution combustion synthesis and characterized by scanning electron microscopy (SEM), X-ray photoemission spectroscopy (XPS), X-ray absorption near-edge spectroscopy (XANES), X-ray diffraction (XRD), and Raman techniques. Overall, our positive electrodes based on Li1.25Mn0.625Ni0.125O2 overlithiated Co-free LRLO is a step forward in the development of the materials for batteries with improved performance and better environmental fingerprint.