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Anion Redox Chemistry in the Cobalt Free 3d Transition Metal Oxide Intercalation Electrode Li[Li0.2Ni0.2Mn0.6]O-2
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- Luo, Kun (author)
- Univ Oxford, Dept Mat, Parks Rd, Oxford OX1 3PH, England.;Univ Oxford, Dept Chem, Parks Rd, Oxford OX1 3PH, England.
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- Roberts, Matthew R. (author)
- Univ Oxford, Dept Mat, Parks Rd, Oxford OX1 3PH, England.;Univ Oxford, Dept Chem, Parks Rd, Oxford OX1 3PH, England.
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- Guerrini, Niccolo (author)
- Univ Oxford, Dept Mat, Parks Rd, Oxford OX1 3PH, England.;Univ Oxford, Dept Chem, Parks Rd, Oxford OX1 3PH, England.
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- Univ Oxford, Dept Mat, Parks Rd, Oxford OX1 3PH, England;Univ Oxford, Dept Chem, Parks Rd, Oxford OX1 3PH, England. Molekyl- och kondenserade materiens fysik (creator_code:org_t)
- 2016-08-24
- 2016
- English.
- In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 138:35, s. 11211-11218
- Journal article (peer-reviewed)
Abstract
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- 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.
Subject headings
- NATURVETENSKAP -- Fysik -- Den kondenserade materiens fysik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Condensed Matter Physics (hsv//eng)
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- Pickup, David M.
- Ramos, Silvia
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