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Charge-compensation in 3d-transition-metal-oxide intercalation cathodes through the generation of localized electron holes on oxygen
Univ Oxford, Dept Mat & Chem, Parks Rd, Oxford OX1 3PH, England..
Univ Oxford, Dept Mat & Chem, Parks Rd, Oxford OX1 3PH, England..
Univ Oxford, Dept Mat & Chem, Parks Rd, Oxford OX1 3PH, England..
Univ Oxford, Dept Mat & Chem, Parks Rd, Oxford OX1 3PH, England..
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2016 (English)In: Nature Chemistry, ISSN 1755-4330, E-ISSN 1755-4349, Vol. 8, no 7, 684-691 p.Article in journal (Refereed) Published
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Abstract [en]

During the charging and discharging of lithium-ion-battery cathodes through the de-and reintercalation of lithium ions, electroneutrality is maintained by transition-metal redox chemistry, which limits the charge that can be stored. However, for some transition-metal oxides this limit can be broken and oxygen loss and/or oxygen redox reactions have been proposed to explain the phenomenon. We present operando mass spectrometry of O-18-labelled Li-1.2[Ni0.132+Co0.133+Mn0.544+]O-2, which demonstrates that oxygen is extracted from the lattice on charging a Li-1.2[Ni0.132+Co0.133+Mn0.544+]O-2 cathode, although we detected no O-2 evolution. Combined soft X-ray absorption spectroscopy, resonant inelastic X-ray scattering spectroscopy, X-ray absorption near edge structure spectroscopy and Raman spectroscopy demonstrates that, in addition to oxygen loss, Li+ removal is charge compensated by the formation of localized electron holes on O atoms coordinated by Mn4+ and Li+ ions, which serve to promote the localization, and not the formation, of true O-2(2-)( peroxide, O-O similar to 1.45 angstrom) species. The quantity of charge compensated by oxygen removal and by the formation of electron holes on the O atoms is estimated, and for the case described here the latter dominates.

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2016. Vol. 8, no 7, 684-691 p.
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Physical Chemistry
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URN: urn:nbn:se:uu:diva-299560DOI: 10.1038/NCHEM.2471ISI: 000378280400012PubMedID: 27325095OAI: oai:DiVA.org:uu-299560DiVA: diva2:949806
Available from: 2016-07-25 Created: 2016-07-22 Last updated: 2016-07-25Bibliographically approved

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