Characterization of Layered Lithium Nickel Manganese Oxides Synthesized by a Novel Oxidative Coprecipitation Method and Their Electrochemical Performance as Lithium Insertion Electrode Materials

Lithium nickel manganese oxides, , (0 ⩽ y ⩽ 0.5) were prepared via a new solution technique. The corresponding mixed nickel manganese hydroxide precursors were synthesized in an oxidative coprecipitation method. Subsequent calcination in the presence of LiOH leads to crystalline products with a partially disordered layered‐type structure. X‐ray photoelectron spectroscopic analysis has indicated a strong enrichment of lithium at the surface. The electrochemical performance of these materials as positive electrodes in lithium‐ion batteries was evaluated as a function of the calcination temperature and manganese content. A calcination temperature of 700°C leads to the best cycling stability. At this temperature, a sufficiently high degree of crystallinity was achieved, having a strong influence on the cycling stability of these "4 V" materials. The specific charge and cycling stability obtained for the solution‐prepared pure lithium nickel oxide, , was low, but was significantly enhanced by replacing some nickel with manganese. With increasing manganese content, the specific charge increased to about for materials with a Ni:Mn ratio of about 1:1. Ex situ magnetic susceptibility measurements proved that during lithium deinsertion, the trivalent manganese is preferentially oxidized, and seems to be the more reactive redox center in these oxides.