Nickel-rich layered LiNi0.8Mn0.1Co0.1O2 with dual gradients on both primary and secondary particles in lithium-ion batteries

The Li+/Ni2+ mixing in LiNi0.8Mn0.1Co0.1O2 (NMC811) leads to fast battery capacity decay. Here we report a dual-gradient nickel-rich layered cathode material (D-NMC 811), using nickel-based metal organic framework of Ni-MOF-74. The formation of a protective layer with rock salt phase due to the reduced nickel oxidation state on the surface of the primary particles resists internal strain and suppresses further phase transition, thus alleviating crack generation. After 300 cycles at 1/3 C, a high half-cell capacity retention of 88.50% with 0.038% decay per cycle is observed. The full-cell battery displays a high capacity retention of >86.7% with a Coulombic efficiency of >99.86% at 1/3 C after 300 cycles. The 300 mAh pouch cell delivers an energy density of 216.4 Wh/kg. After 500 cycles at 1.0 C, it still displays 84.1% capacity retention while the battery with conventional NMC811 only shows a retention of 53.0% after 400 cycles.