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High reversibility of lattice oxygen redox quantified by direct bulk probes of both anionic and cationic redox reactions
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(2019) High reversibility of lattice oxygen redox quantified by direct bulk probes of both anionic and cationic redox reactions. Joule, 3 (2). pp. 518-541. doi:10.1016/j.joule.2018.11.014 ISSN 2542-4351.
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Official URL: http://dx.doi.org/10.1016/j.joule.2018.11.014
Abstract
The reversibility and cyclability of anionic redox in battery electrodes hold the key to its practical employments. Here, through mapping of resonant inelastic X-ray scattering (mRIXS), we have independently quantified the evolving redox states of both cations and anions in Na2/3Mg1/3Mn2/3O2. The bulk Mn redox emerges from initial discharge and is quantified by inverse partial fluorescence yield (iPFY) from Mn-L mRIXS. Bulk and surface Mn activities likely lead to the voltage fade. O-K super-partial fluorescence yield (sPFY) analysis of mRIXS shows 79% lattice oxygen redox reversibility during the initial cycle, with 87% capacity sustained after 100 cycles. In Li1.17Ni0.21Co0.08Mn0.54O2, lattice oxygen redox is 76% initial-cycle reversible but with only 44% capacity retention after 500 cycles. These results unambiguously show the high reversibility of lattice oxygen redox in both Li-ion and Na-ion systems. The contrast between Na2/3Mg1/3Mn2/3O2 and Li1.17Ni0.21Co0.08Mn0.54O2 systems suggests the importance of distinguishing lattice oxygen redox from other oxygen activities for clarifying its intrinsic properties.
Item Type: | Journal Article | ||||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) | ||||||||
Journal or Publication Title: | Joule | ||||||||
Publisher: | Elsevier | ||||||||
ISSN: | 2542-4351 | ||||||||
Official Date: | 20 February 2019 | ||||||||
Dates: |
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Volume: | 3 | ||||||||
Number: | 2 | ||||||||
Page Range: | pp. 518-541 | ||||||||
DOI: | 10.1016/j.joule.2018.11.014 | ||||||||
Status: | Peer Reviewed | ||||||||
Publication Status: | Published | ||||||||
Access rights to Published version: | Restricted or Subscription Access |
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