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

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 Li 1.17Ni 0.21Co 0.08Mn 0.54O 2 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 Li 1.17Ni 0.21Co0.08Mn 0.54O 2 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,more » analysis, and theoretical calculation for probing and understanding oxygen redox reactions.« less

Authors:
 [1];  [2];  [3];  [4]; ORCiD logo [1];  [5];  [6];  [7]; ORCiD logo [7]
  1. Stanford Univ., Stanford, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Shandong Univ., Jinan (China)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Binghamton Univ., Binghamton, NY (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Peking Univ. Shenzhen Graduate School, Shenzhen (China)
  5. Stanford Univ., Stanford, CA (United States)
  6. Shandong Univ., Jinan (China)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1564071
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Condensed Matter
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2410-3896
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
oxygen redox; battery electrode; layered oxide; Li-ion battery; resonant inelastic X-ray scattering

Citation Formats

Wu, Jinpeng, Li, Qinghao, Sallis, Shawn, Zhuo, Zengqing, Gent, William E., Chueh, William C., Yan, Shishen, Chuang, Yi-de, and Yang, Wanli. Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering. United States: N. p., 2019. Web. doi:10.3390/condmat4010005.
Wu, Jinpeng, Li, Qinghao, Sallis, Shawn, Zhuo, Zengqing, Gent, William E., Chueh, William C., Yan, Shishen, Chuang, Yi-de, & Yang, Wanli. Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering. United States. doi:10.3390/condmat4010005.
Wu, Jinpeng, Li, Qinghao, Sallis, Shawn, Zhuo, Zengqing, Gent, William E., Chueh, William C., Yan, Shishen, Chuang, Yi-de, and Yang, Wanli. Sat . "Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering". United States. doi:10.3390/condmat4010005. https://www.osti.gov/servlets/purl/1564071.
@article{osti_1564071,
title = {Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering},
author = {Wu, Jinpeng and Li, Qinghao and Sallis, Shawn and Zhuo, Zengqing and Gent, William E. and Chueh, William C. and Yan, Shishen and Chuang, Yi-de and Yang, Wanli},
abstractNote = {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.},
doi = {10.3390/condmat4010005},
journal = {Condensed Matter},
number = 1,
volume = 4,
place = {United States},
year = {2019},
month = {1}
}

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