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Seo DH, Lee J, Urban A, et al. The structural and chemical origin of the oxygen redox activity in layered and cation-disordered Li-excess cathode materials. Nat Chem. 2016;8(7):692-7doi: 10.1038/nchem.2524.
Seo, D. H., Lee, J., Urban, A., Malik, R., Kang, S., & Ceder, G. (2016). The structural and chemical origin of the oxygen redox activity in layered and cation-disordered Li-excess cathode materials. Nature chemistry, 8(7), 692-7. https://doi.org/10.1038/nchem.2524
Seo, Dong-Hwa, et al. "The structural and chemical origin of the oxygen redox activity in layered and cation-disordered Li-excess cathode materials." Nature chemistry vol. 8,7 (2016): 692-7. doi: https://doi.org/10.1038/nchem.2524
Seo DH, Lee J, Urban A, Malik R, Kang S, Ceder G. The structural and chemical origin of the oxygen redox activity in layered and cation-disordered Li-excess cathode materials. Nat Chem. 2016 Jul;8(7):692-7. doi: 10.1038/nchem.2524. Epub 2016 May 30. PMID: 27325096.
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Nat Chem. 2016 Jul;8(7):692-7. doi: 10.1038/nchem.2524. Epub 2016 May 30.

The structural and chemical origin of the oxygen redox activity in layered and cation-disordered Li-excess cathode materials.

Nature chemistry

Dong-Hwa Seo, Jinhyuk Lee, Alexander Urban, Rahul Malik, ShinYoung Kang, Gerbrand Ceder

Affiliations

  1. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
  2. Department of Materials Science and Engineering, UC Berkeley, Berkeley, California 94720, USA.
  3. Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.

PMID: 27325096 DOI: 10.1038/nchem.2524

Abstract

Lithium-ion batteries are now reaching the energy density limits set by their electrode materials, requiring new paradigms for Li(+) and electron hosting in solid-state electrodes. Reversible oxygen redox in the solid state in particular has the potential to enable high energy density as it can deliver excess capacity beyond the theoretical transition-metal redox-capacity at a high voltage. Nevertheless, the structural and chemical origin of the process is not understood, preventing the rational design of better cathode materials. Here, we demonstrate how very specific local Li-excess environments around oxygen atoms necessarily lead to labile oxygen electrons that can be more easily extracted and participate in the practical capacity of cathodes. The identification of the local structural components that create oxygen redox sets a new direction for the design of high-energy-density cathode materials.

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