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

Journal Article · · Condensed Matter
 [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)

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1564071
Journal Information:
Condensed Matter, Vol. 4, Issue 1; ISSN 2410-3896
Publisher:
MDPICopyright Statement
Country of Publication:
United States
Language:
English

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