Regensburg 2025 – scientific programme

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KFM: Fachverband Kristalline Festkörper und deren Mikrostruktur

KFM 7: Materials for the Storage and Conversion of Energy (joint session MM/KFM)

KFM 7.3: Talk

Monday, March 17, 2025, 17:45–18:00, H22

Insights into Li-ion battery cathode redox chemistry via charge transfer multiplet simulations of LiNi_1/3Mn_1/3Co_1/3O₂ — •Ruiwen Xie¹, Maximilian Mellin², Wolfram Jaegermann², Jan. P Hofmann², and Hongbin Zhang¹ — ¹Theory of Magnetic Materials Group, Department of Materials and Geosciences, Technical University of Darmstadt — ²Surface Science Laboratory, Department of Materials and Geosciences, Technical University of Darmstadt

The evolution of electronic structure during discharging and charging processes with Li intercalation and deintercalation in transition metal oxide cathode materials involves changes in oxidation states, non-rigid band behavior, and oxygen’s role in charge compensation, which significantly impact cathode performance. To gain deeper insights, we combine experimental x-ray photoelectron spectroscopy (XPS) at various voltages with many-body electronic structure simulations. The electronic structures of Li_xCoO₂ and Li_xNiO₂ were calculated using Density Functional Theory and Dynamical Mean-Field Theory (DFT+DMFT). We found that Li intercalation and deintercalation shift the hybridization between Co/Ni d and O p orbitals relative to the Fermi energy, altering Co/Ni d occupancy. Based on this, we performed XPS calculations using the multiplet ligand-field model in Quanty to revisit the transition metal 2p satellite structure evolution. This study provides crucial insights into the interplay between electronic structure and Li intercalation dynamics for enhancing cathode performance.

Keywords: Cathode materials; X-ray photoelectron spectroscopy (XPS); Redox chemistry; Electronic structure; Multiplet ligand-field model