Exposing the {010} Planes by Oriented Self-Assembly with Nanosheets to Improve the Electrochemical Performances of Ni-Rich Li[Ni_0.8Co_0.1Mn_0.1]O₂ Microspheres

A modified Ni-rich Li[Ni_0.8Co_0.1Mn_0.1]O₂ cathode material with exposed {010} planes is successfully synthesized for lithium-ion batteries. The scanning electron microscopy images have demonstrated that by tuning the ammonia concentration during the synthesis of precursors, the primary nanosheets could be successfully stacked along the [001] crystal axis predominantly, self-assembling like multilayers. According to the high-resolution transmission electron microscopy results, such a morphology benefits the growth of the {010} active planes of final layered cathodes during calcination treatment, resulting in the increased area of the exposed {010} active planes, a well-ordered layer structure, and a lower cation mixing disorder. The Li-ion diffusion coefficient has also been improved after the modification based on the results of potentiostatic intermittent titration technique. As a consequence, the modified Li[Ni_0.8Co_0.1Mn_0.1]O₂ material exhibits superior initial discharges of 201.6 mA h g^-1 at 0.2 C and 185.7 mA h g^-1 at 1 C within 2.8-4.3 V (vs Li⁺/Li), and their capacity retentions after 100 cycles reach 90 and 90.6%, respectively. The capacity at 10 C also increases from 98.3 to 146.5 mA h g^-1 after the modification. Our work proposes a novel approach for exposing high-energy {010} active planes of the layered cathode material and again confirms its validity in improving electrochemical properties.