Impact of Hybridization and Correlations on Transition-Metal Valence and Oxygen Redox in Li-ion Battery Cathode Materials

ORAL

Abstract

Transition-metal oxide battery cathode compounds undergo distinct changes in their electronic distribution as one goes from a fully lithiated to a fully delithiated state. This would lead nominally to energetically unfavorable high valence states on the transition-metal, affecting overall energy capacity. Here, we analyze the influence of metal-to-ligand orbital hybridization and effective charge transfer using a configuration interaction cluster model to simulate different spectroscopic tools. We connect our observations to the framework of anionic redox, which prevents high transition-metal valency, and has been linked to increases in energy capacity of Li-ion batteries. By gaining insight into crucial features that are identified with such processes, we aim to have a greater understanding of the fundamental physics of Li-ion cathode materials, in the hopes of predicting novel, better performing Li-ion compounds.

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Presenters

  • Ilkyu Lee

    • Stanford University

Authors

  • Ilkyu Lee

    • Stanford University

  • Chunjing Jia

    • Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory
    • SIMES, SLAC National Accelerator Lab
    • SSRL Materials Science Division, SLAC National Accelerator Laboratory and Stanford University
    • Stanford University

  • Brian Moritz

    • Stanford University
    • Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory
    • SLAC National Accelerator Laboratory
    • SLAC and Stanford University
    • Institute for Materials and Energy Science, Stanford
    • SSRL Materials Science Division, SLAC National Accelerator Laboratory and Stanford University

  • Thomas Devereaux

    • Stanford University
    • Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory
    • SLAC National Accelerator Laboratory
    • Physics, Stanford University
    • SLAC and Stanford University
    • Institute for Materials and Energy Science, Stanford
    • SIMES, SLAC National Accelerator Lab
    • SLAC National Accelerator Laboratory and Stanford University, Stanford Institute for Materials and Energy Sciences
    • SLAC, Stanford
    • SIMES, SLAC, and Stanford University
    • Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory and Stanford University