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Energy density limitations of layered oxides with different Ni contents,i.e., of the conventional cathode materials in Li-ion batteries, areinvestigated across the first discharge cycle using advanced spectroscopy andstate-of-the-art diffraction. For the first time unambiguous experimentalevidence is provided, that redox reactions in NCMs proceed via a reversibleoxidation of Ni and a hybridization with O, and not, as widely assumed, viapure cationic or more recently discussed, pure anionic redox processes. OnceNi-O hybrid states are formed, the sites cannot be further oxidized. Instead,irreversible reactions set in which lead to a structural collapse and thus, thelack of ionic Ni limits the reversible capacity. Moreover, the degree ofhybridization, which varies with the Ni content, triggers the electronicstructure and the operation potential of the cathodes. With an increasingamount of Ni, the covalent character of the materials increases and thepotential decreases.

On the microscopic origin of reversible and irreversible reactions of  LiNixCoyMnx cathode materials: Ni-O hybrid bond formation vs. cationic and  anionic redox