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First-cycle voltage hysteresis in Li-rich 3d cathodes associated with molecular O2 trapped in the bulk
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House, Robert A., Rees, Gregory J., Pérez-Osorio, Miguel A., Marie, John-Joseph, Boivin, Edouard, Robertson, Alex W., Nag, Abhishek, Garcia-Fernandez, Mirian, Zhou, Ke-Jin and Bruce, Peter G. (2020) First-cycle voltage hysteresis in Li-rich 3d cathodes associated with molecular O2 trapped in the bulk. Nature Energy, 5 (10). pp. 777-785. doi:10.1038/s41560-020-00697-2 ISSN 2058-7546.
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Official URL: http://dx.doi.org/10.1038/s41560-020-00697-2
Abstract
Li-rich cathode materials are potential candidates for next-generation Li-ion batteries. However, they exhibit a large voltage hysteresis on the first charge/discharge cycle, which involves a substantial (up to 1 V) loss of voltage and therefore energy density. For Na cathodes, for example Na0.75[Li0.25Mn0.75]O2, voltage hysteresis can be explained by the formation of molecular O2 trapped in voids within the particles. Here we show that this is also the case for Li1.2Ni0.13Co0.13Mn0.54O2. Resonant inelastic X-ray scattering and 17O magic angle spinning NMR spectroscopy show that molecular O2, rather than O22−, forms within the particles on the oxidation of O2− at 4.6 V versus Li+/Li on charge. These O2 molecules are reduced back to O2− on discharge, but at the lower voltage of 3.75 V, which explains the voltage hysteresis in Li-rich cathodes. 17O magic angle spinning NMR spectroscopy indicates a quantity of bulk O2 consistent with the O-redox charge capacity minus the small quantity of O2 loss from the surface. The implication is that O2, trapped in the bulk and lost from the surface, can explain O-redox.
Item Type: | Journal Article | ||||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||
Journal or Publication Title: | Nature Energy | ||||||||
Publisher: | Nature Publishing Group | ||||||||
ISSN: | 2058-7546 | ||||||||
Official Date: | 21 September 2020 | ||||||||
Dates: |
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Volume: | 5 | ||||||||
Number: | 10 | ||||||||
Page Range: | pp. 777-785 | ||||||||
DOI: | 10.1038/s41560-020-00697-2 | ||||||||
Status: | Peer Reviewed | ||||||||
Publication Status: | Published | ||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||
Copyright Holders: | The Author(s), under exclusive licence to Springer Nature Limited | ||||||||
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