Full concentration gradient (FCG) cathode material having nickel-rich core Li [Ni 0.89 Rechargeable lithium-ion batteries have received great attention as power sources for portable electronic device, plug-in hybrid vehicles (PHEVs), and electric vehicles (EVs) because of their high energy density, long cycle life, and excellent rate capability. However, commercialization of rechargeable lithium-ion battery system for the automobile industry requires further improvements in energy density and safety. In order to meet these requirements, numerous researches have been in progress for finding new electrode materials, especially cathode materials.1-4 So far, most of the studies have focused on the layered cathode materials, Li[Ni 1−y−z Co y Mn z ]O 2 , which combine the rate performance of LiCoO 2 , the high capacity of LiNiO 2 , and the structural stability imparted by the presence of Mn 4+ . 5 Particularly, the Ni-rich layered composite oxides Li[Ni 1−y−z Co y Mn z ]O 2 (1-y-z ≥ 0.8), are considered one of the most promising cathode materials because they offer higher capacity than currently commercialized cathode materials. 6,7 However, the Ni-rich materials have poor thermal stability due to the oxygen release at the charged state, which can lead to severe thermal runaway and possible explosion. [8][9][10] Moreover, the unstable Ni 4+ ions can be easily reduced to inactive NiO, resulting in increase of the interfacial impedance, and thus poor cycle life.
11,12To overcome these problems of the Ni-rich Li[Ni 1−y−z Co y Mn z ]O 2 layered cathode materials, we have developed a functional lithium nickel-cobalt-manganese oxide cathode material which have coreshell structure or core-shell with concentration gradient. These cathodes are composed of a Mn-rich outer surface providing the outstanding safety and a Ni-rich core delivering a high capacity. These cathodes show high capacity and good cycle life at high voltage cycling, and improved safety characteristics.3,13,14 Recently, we reported a highenergy cathode material with a full concentration gradient (FCG) of Ni, Co, and Mn ions consisting of rod-shaped primary particles grown in radial directions with a crystallographic texture, which improved the rate capability and safety characteristics. 15 Based on the proposed material design concept, we can design various cathode materials with different gradient compositions.In this study, we report newly designed FCG Li [Ni 0.65
ExperimentalThe FCG precursors were synthesized through the co-precipitation method.15 The Ni-poor aqueous solution (Ni:Co:Mn = 0.58:0.10:0.32 in molar ratio) from tank 2was slowly pumped into a Ni-rich aqueous solution (Ni:Mn=0.96:0.04 in molar ratio) in tank 1. The homogeneous mixture was then fed into a continuously stirred tank reactor (CSTR). At the same time, a 4.0 mol dm −3 solution of NaOH (aq.) and the desired amount of NH 4 OH solution (aq.) (chelating agent) under N 2 atmosphere were also separately pumped into the reactor. The molar ratio of ammonium hydroxide to transition metal...