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Irreversible anion oxidation leads to dynamic charge compensation in the Ru-poor, Li-rich cathode Li2Ru0.3Mn0.7O3
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Zak, Joshua J., Zuba, Mateusz, Lebens-Higgins, Zachary W., Huang, Heran, Crafton, Matthew J., Dalleska, Nathan F., McCloskey, Bryan D., Piper, Louis F. J. and See, Kimberly A. (2023) Irreversible anion oxidation leads to dynamic charge compensation in the Ru-poor, Li-rich cathode Li2Ru0.3Mn0.7O3. ACS Energy Letters, 8 . pp. 722-730. doi:10.1021/acsenergylett.2c02537 ISSN 2380-8195.
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WRAP-Irreversible-anion-oxidation-leads-to-dynamic-charge-compensation-in-the-Ru-poor-Li-rich-cathode-Li2Ru0.3Mn0.7O3-Piper-2023.pdf - Accepted Version - Requires a PDF viewer. Download (5Mb) | Preview |
Official URL: https://doi.org/10.1021/acsenergylett.2c02537
Abstract
Conventional cathodes for Li-ion batteries are layered transition-metal oxides that support Li+ intercalation charge-balanced by redox on the transition metals. Oxidation beyond one electron per transition metal can be achieved in Li-rich layered oxides by involving structural anions, which necessitates high voltages and complex charge compensation mechanisms convoluted by degradation reactions. We report a detailed structural and spectroscopic analysis of the multielectron material Li2Ru0.3Mn0.7O3, chosen due to its low Ru content. Ex situ and operando spectroscopic data over multiple cycles highlight the changing charge compensation mechanism. Notably, over half of the first-cycle capacity is attributed to O2 gas evolution and reversible O redox is minimal. Instead, reduced Ru and Mn species are detected in the bulk and on the surface, which then increasingly contribute to charge compensation as more metal reduction occurs with cycling. Permanent structural changes linked to metal migration are observed with EXAFS and Raman analysis.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QD Chemistry T Technology > TK Electrical engineering. Electronics Nuclear engineering |
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Divisions: | Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) | ||||||||||||
SWORD Depositor: | Library Publications Router | ||||||||||||
Library of Congress Subject Headings (LCSH): | Cathodes, Lithium compounds -- Oxidation, Lithium ion batteries -- Materials, Anions | ||||||||||||
Journal or Publication Title: | ACS Energy Letters | ||||||||||||
Publisher: | American Chemical Society | ||||||||||||
ISSN: | 2380-8195 | ||||||||||||
Official Date: | January 2023 | ||||||||||||
Dates: |
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Volume: | 8 | ||||||||||||
Page Range: | pp. 722-730 | ||||||||||||
DOI: | 10.1021/acsenergylett.2c02537 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||||
Copyright Holders: | American Chemical Society | ||||||||||||
Date of first compliant deposit: | 9 January 2023 | ||||||||||||
Date of first compliant Open Access: | 28 December 2023 | ||||||||||||
RIOXX Funder/Project Grant: |
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