h i g h l i g h t s g r a p h i c a l a b s t r a c tA cathode material combining Nirich and Li-rich phase was developed.The existence of Li-rich phase improves the surface chemical stability. Li-rich ordering is observed in layered oxide with Ni-rich (x > 0.5) rather than Mn-rich (y > 0.5). Excellent cycle performance is achieved in both half and pouch-type full cell.
a b s t r a c tA facile synthesis method has been developed to prepare xLi 2 MnO 3 $(1Àx)LiNi 0.7 Co 0.15 Mn 0.15 O 2 (x ¼ 0, 0.03, 0.07, 0.10, 0.20, and 0.30) cathode materials, combining the advantages of the high specific capacity of the Ni-rich layered phase and the surface chemical stability of the Li-rich layered phase. X-ray diffraction (XRD), transmission electron microscopy (TEM), and electrochemical charge/discharge measurements confirm the formation of a Li-rich layered phase with C2/m symmetry. The high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) reveals a spatial relationship that the Li-rich nano-domain islands are integrated into the conventional Ni-rich layered matrix (R3m). Most importantly, this is the first time that Li-rich phase has been directly observed inside a particle at the nano-scale, when the overall composition of the layered oxide Li 1þd Ni 1ÀyÀzÀd Mn y M z O 2 (M ¼ metal) is Nirich (>0.5) rather than Mn-rich (>0.5). Remarkably, the xLi 2 MnO 3 $(1Àx)LiNi 0.7 Co 0.15 Mn 0.15 O 2 cathodes with optimized x value shows superior electrochemical performance at C/3 rate: an initial capacity of 190 mA h g À1 with 90% capacity retention after 400 cycles in a half cell and 73.5% capacity retention after 900 cycles in a pouch-type full cell.