Li-ion batteries are at the frontier of energy storage devices. Layered transition metal oxides, particularly Co-free cathodes, are being investigated due to their low cost yet high theoretical energy density. The challenge with using oxide cathodes is their inherent surface structure and electronic instability caused by metal cation migration into Li-sites via a phenomenon known as surface reconstruction. During charging, the redox center becomes oxidized further generating thermodynamically favorable electron transfer pathways between the electrolyte and oxide cathode due to TM3d-O2p orbital hybridization perturbation during cycling. The cathode-electrolyte interface leads to various undesired electrolyte degradation pathways that can minimize coulombic efficiency. Electrolyte degradation occurs at the oxide cathode surface, but it can lead to bulk electronic and structural changes. At varying states-of-charge electrolyte degradation could potentially promote greater chemomechanical breakdown and irreversible phase transformations at different C-rates. In this study, we focus on understanding the interplay between bulk phase transformations and surface instability to understand how states-of-charge impact electrolyte degradation kinetics. We modify electrolyte systems to understand the impact of different organic species. By using proposed voltage oscillation experiments, electron microscopy, and synchotron X-Ray techniques, we will probe the interfacial chemistry in Co-free systems.

Understanding the relationship between oxide cathode charge state and electrolyte degradation pathways

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.