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Anion Redox Chemistry in the Cobalt Free 3d Transition Metal Oxide Intercalation Electrode Li[Li0.2Ni0.2Mn0.6]O-2

Journal of the American Chemical Society, 2016-09, Vol.138 (35), p.11211 [Peer Reviewed Journal]

ISSN: 1520-5126 ;ISSN: 0002-7863 ;EISSN: 1520-5126 ;DOI: 10.1021/jacs.6b05111

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  • Title:
    Anion Redox Chemistry in the Cobalt Free 3d Transition Metal Oxide Intercalation Electrode Li[Li0.2Ni0.2Mn0.6]O-2
  • Author: Luo, Kun ; Roberts, Matthew R. ; Guerrini, Niccolo ; Tapia-Ruiz, Nuria ; Hao, Rong ; Massel, Felix ; Pickup, David M. ; Ramos, Silvia ; Liu, Yi-Sheng ; Guo, Jinghua ; Chadwick, Alan V. ; Duda, Laurent C. ; Bruce, Peter G.
  • Is Part Of: Journal of the American Chemical Society, 2016-09, Vol.138 (35), p.11211
  • Description: Conventional intercalation cathodes for lithium batteries store charge in redox reactions associated with the transition metal cations, e.g., Mn3+/4+ in LiMn2O4, and this limits the energy storage of Li-ion batteries. Compounds such as Li[Li0.2Ni0.2Mn0.6]O-2 exhibit a capacity to store charge in excess of the transition metal redox reactions. The additional capacity occurs at and above 4.5 V versus Li+/Li. The capacity at 4.5 V is dominated by oxidation of the O-2(-) anions accounting for similar to 0.43 e(-)/formula unit, with an additional 0.06 e(-)/formula unit being associated with O loss from the lattice. In contrast, the capacity above 4.5 V is mainly O loss, similar to 0.08 e(-)/formula. The O redox reaction involves the formation of localized hole states on O during charge, which are located on O coordinated by (Mn4+/Li+). The results have been obtained by combining operando electrochemical mass spec on 180 labeled Li[Li0.2Ni0.2Mn0.6]O-2 with XANES, soft X-ray spectroscopy, resonant inelastic X-ray spectroscopy, and Raman spectroscopy. Finally the general features of O redox are described with discussion about the role of comparatively ionic (less covalent) 3d metal oxygen interaction on anion redox in lithium rich cathode materials.
  • Language: English
  • Identifier: ISSN: 1520-5126
    ISSN: 0002-7863
    EISSN: 1520-5126
    DOI: 10.1021/jacs.6b05111
  • Source: SWEPUB Freely available online
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