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The present work reviews the charge compensation in Ni based layered oxides(LiNi1-xMexO2 with x <= 0.2, Me = Co, Mn, space group R-3m) relatingperformance parameters to changes in the electronic and crystallographicstructure of the cathode materials. Upon charge and discharge two fundamentallydifferent redox mechanisms are observed: At low and medium states of charge(SOCs) charge compensation takes mainly place at oxygen sites while electrondensity is shifted from the oxygen lattice to nickel (formation of sigmabonds). At high SOCs the shift of electron density from the transition metalsto oxygen (formation of pi bonds) enables an additional redox process but alsooxygen release from the transition metal host structure and subsequentdetrimental reactions. Depending on the Ni:Co:Mn content, both processes leadto characteristic features in the voltage profile of the cathode materials andperformance parameters like the capacity, the cycling stability and the opencell voltage become a function of the composition.

A review and outlook on anionic and cationic redox in Ni-, Li- and Mn-rich layered oxides LiMeO2 (Me = Li, Ni, Co, Mn)