Ni-rich
layered oxides Li[Ni
x
Co
y
Al1–x–y
]O2 (NCA) have become
the state-of-the-art
cathode materials for high-energy-density Li-ion batteries (LIBs).
However, the solubility product of Al(OH)3 is much lower
than that of Ni(OH)2 and Co(OH)2, which makes
it difficult to produce the NCA precursor with a stoichiometric amount
and uniform distribution of Al element in one step by using the coprecipitation
method. In addition, high temperatures or complex procedures are required
to obtain the single-crystalline Ni-rich cathode materials from the
coprecipitation-derived precursor. Here, we develop a modified cation
chelation and reassembly process to produce the stoichiometric NCA
precursor in a single step. During this process, the addition of acetic
acid causes Ni, Co, and Al species to exist in solution as free metal
ions instead of hydroxide precipitates, which can be efficiently chelated
by ethylenediaminetetraacetic acid and then reassembled into the crystalline
precursor. After the lithiation treatment at 500 °C for 6 h and
750 °C for 12 h, the obtained single-crystalline NCA cathode
exhibits a high discharge capacity (203.1 mA h g–1 at 0.1C between 3.0 and 4.3 V), good cycling stability (87.2% capacity
retention after 100 cycles), and excellent rate capability (126.5
mA h g–1 at 10C). The outstanding electrochemical
performance can be attributed to the cooperation of the single crystal
together with the stoichiometric amount and uniform distribution of
Al element, which can suppress the Li+/Ni2+ mixing
level and stabilize the layer structure, enabling fast Li+ diffusivity and electronic conductivity.