A novel hierarchical precursor of densely integrated hydroxide nanoflakes on oxide microspheres toward high-performance layered Ni-rich cathode for lithium ion batteries

Abstract

Herein, a novel hierarchical precursor of Ni_0.8Co_0.1Mn_0.1O_x@Ni_0.8Co_0.1Mn_0.1(OH)₂ is proposed for the first time, which was synthesized by densely integrating co-precipitated Ni_0.8Co_0.1Mn_0.1(OH)₂ nanoflakes onto spray-pyrolyzed Ni_0.8Co_0.1Mn_0.1O_x microspheres. The co-precipitated hydroxide layer can prevent the Ni_0.8Co_0.1Mn_0.1O_x microspheres from fragmenting during the sintering process, thus yielding uniform LiNi_0.8Co_0.1Mn_0.1O₂ spheres with a hollow interior morphology. Strikingly, the obtained spherical LiNi_0.8Co_0.1Mn_0.1O₂ cathode exhibits improved tap density and initial coulombic efficiency, as well as excellent cycling stability and superior rate capability. Discharge capacities of 169 mA h g⁻¹ after 300 cycles at 1C (180 mA g⁻¹) of between 2.8 and 4.3 V are consistently obtained, corresponding to 90.5% capacity retention. Significantly, it is strongly envisioned that this novel hierarchical structure design concept holds great promise for the architectural construction of other energy storage materials.