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Layered LiMO2 (M = Ni, Co, Mn, and Al mixture) cathode materials used forLi-ion batteries are reputed to be highly reactive through their surface, wherethe chemistry changes rapidly when exposed to ambient air. However,conventional electron/spectroscopy-based techniques or thermogravimetricanalysis fails to capture the underlying atom-scale chemistry of vulnerable Lispecies. To study the evolution of the surface composition at the atomic scale,here we use atom probe tomography and probed the surface species formed duringexposure of a LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode material to air. Thecompositional analysis evidences the formation of Li2CO3. Site specificexamination from a cracked region of an NMC811 particle also suggests thepredominant presence of Li2CO3. These insights will help to design improvedprotocols for cathode synthesis and cell assembly, as well as criticalknowledge for cathode degradation

Atomic scale evolution of the surface chemistry in Li[Ni,Mn,Co]O2 cathode for Li-ion batteries stored in air