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

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,...

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Main Authors: Jinpeng Wu, Qinghao Li, Shawn Sallis, Zengqing Zhuo, William E. Gent, William C. Chueh, Shishen Yan, Yi-de Chuang, Wanli Yang
Format: Article
Language:English
Published: MDPI AG 2019-01-01
Series:Condensed Matter
Subjects:
Online Access:http://www.mdpi.com/2410-3896/4/1/5
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author Jinpeng Wu
Qinghao Li
Shawn Sallis
Zengqing Zhuo
William E. Gent
William C. Chueh
Shishen Yan
Yi-de Chuang
Wanli Yang
author_facet Jinpeng Wu
Qinghao Li
Shawn Sallis
Zengqing Zhuo
William E. Gent
William C. Chueh
Shishen Yan
Yi-de Chuang
Wanli Yang
author_sort Jinpeng Wu
collection DOAJ
description 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.
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spelling doaj.art-7578784b5797421392047bc0844b3d802022-12-22T04:01:25ZengMDPI AGCondensed Matter2410-38962019-01-0141510.3390/condmat4010005condmat4010005Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray ScatteringJinpeng Wu0Qinghao Li1Shawn Sallis2Zengqing Zhuo3William E. Gent4William C. Chueh5Shishen Yan6Yi-de Chuang7Wanli Yang8Stanford Institute for Materials and Energy Sciences, Stanford University, Stanford, CA 94305, USAAdvanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USAAdvanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USAAdvanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USAStanford Institute for Materials and Energy Sciences, Stanford University, Stanford, CA 94305, USAStanford Institute for Materials and Energy Sciences, Stanford University, Stanford, CA 94305, USASchool of Physics, National Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, ChinaAdvanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USAAdvanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USARealizing 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.http://www.mdpi.com/2410-3896/4/1/5oxygen redoxbattery electrodelayered oxideLi-ion batteryresonant inelastic X-ray scattering
spellingShingle Jinpeng Wu
Qinghao Li
Shawn Sallis
Zengqing Zhuo
William E. Gent
William C. Chueh
Shishen Yan
Yi-de Chuang
Wanli Yang
Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering
Condensed Matter
oxygen redox
battery electrode
layered oxide
Li-ion battery
resonant inelastic X-ray scattering
title Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering
title_full Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering
title_fullStr Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering
title_full_unstemmed Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering
title_short Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering
title_sort fingerprint oxygen redox reactions in batteries through high efficiency mapping of resonant inelastic x ray scattering
topic oxygen redox
battery electrode
layered oxide
Li-ion battery
resonant inelastic X-ray scattering
url http://www.mdpi.com/2410-3896/4/1/5
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