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Condens. Matter 2019, 4(1), 5; https://doi.org/10.3390/condmat4010005

Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering

1
Stanford Institute for Materials and Energy Sciences, Stanford University, Stanford, CA 94305, USA
2
Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USA
3
School of Physics, National Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China
4
Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, NY 13902, USA
5
School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen 518055, China
*
Author to whom correspondence should be addressed.
Received: 15 December 2018 / Revised: 28 December 2018 / Accepted: 29 December 2018 / Published: 5 January 2019
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Abstract

Realizing reversible reduction-oxidation (redox) reactions of lattice oxygen in batteries is a promising way to improve the energy and power density. However, conventional oxygen absorption spectroscopy fails to distinguish the critical oxygen chemistry in oxide-based battery electrodes. Therefore, high-efficiency full-range mapping of resonant inelastic X-ray scattering (mRIXS) has been developed as a reliable probe of oxygen redox reactions. Here, based on mRIXS results collected from a series of Li1.17Ni0.21Co0.08Mn0.54O2 electrodes at different electrochemical states and its comparison with peroxides, we provide a comprehensive analysis of five components observed in the mRIXS results. While all the five components evolve upon electrochemical cycling, only two of them correspond to the critical states associated with oxygen redox reactions. One is a specific feature at 531.0 eV excitation and 523.7 eV emission energy, the other is a low-energy loss feature. We show that both features evolve with electrochemical cycling of Li1.17Ni0.21Co0.08Mn0.54O2 electrodes, and could be used for characterizing oxidized oxygen states in the lattice of battery electrodes. This work provides an important benchmark for a complete assignment of all mRIXS features collected from battery materials, which sets a general foundation for future studies in characterization, analysis, and theoretical calculation for probing and understanding oxygen redox reactions. View Full-Text
Keywords: oxygen redox; battery electrode; layered oxide; Li-ion battery; resonant inelastic X-ray scattering oxygen redox; battery electrode; layered oxide; Li-ion battery; resonant inelastic X-ray scattering
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).
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Wu, J.; Li, Q.; Sallis, S.; Zhuo, Z.; Gent, W.E.; Chueh, W.C.; Yan, S.; Chuang, Y.-D.; Yang, W. Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering. Condens. Matter 2019, 4, 5.

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