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Understanding the role of metal and oxygen in the redox process of layered 3dtransition metal oxides is crucial to build high density and stable nextgeneration Li-ion batteries. We combine hard X-ray photoelectron spectroscopyand ab-initio-based cluster model simulations to study the electronic structureof prototypical end-members LiCoO2 and CoO2. The role of cobalt and oxygen inthe redox process is analyzed by optimizing the values of d-d electronrepulsion and ligand-metal p-d charge transfer to the Co 2p spectra. We clarifythe nature of oxidized cobalt ions by highlighting the transition from positiveto negative ligand-to-metal charge transfer upon Li+ de-intercalation.

Self-regulated ligand-metal charge transfer upon lithium ion de-intercalation process from LiCoO2 to CoO2