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Title: Advances in soft X-ray RIXS for studying redox reaction states in batteries

Abstract

Redox (reduction and oxidation) chemistry provides the fundamental basis for numerous energy-related electrochemical devices. Detecting the electrochemical redox chemistry is pivotal but challenging because it requires independent probes of the cationic and anionic redox states at different electrochemical states. Here, the synchrotron-based soft X-ray mapping of resonant inelastic X-ray scattering (mRIXS) has recently emerged as a powerful tool for exploring such states in electrochemical devices, especially batteries. High-efficiency mRIXS covers the energy range of the absorption edge with the extra dimension of information on the emitted photon energies. In this frontier article, we review recent representative demonstrations of utilizing soft X-ray mRIXS for detecting the novel chemical state during electrochemical operation and for quantifying the cationic redox reactions through inverse partial fluorescence yield analysis (mRIXS-iPFY). More importantly, the non-divalent states of oxygen in electrodes involving oxygen redox reactions could be reliably captured by mRIXS, with its reversibility quantified by the intensity variation of the characteristic mRIXS feature through a super-partial fluorescence yield analysis (mRIXS-sPFY). These recent demonstrations inspire future perspectives on using mRIXS for studying the complex phenomena in energy materials, with both technical and scientific challenges in RIXS theory, in situ/operando experiments, and spatially resolved RIXS imaging.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Xiamen Univ. (China); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Xiamen Univ. (China)
  3. 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)
OSTI Identifier:
1845093
Alternate Identifier(s):
OSTI ID: 1647259
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 49; Journal Issue: 39; Journal ID: ISSN 1477-9226
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wu, Jue, Yang, Yong, and Yang, Wanli. Advances in soft X-ray RIXS for studying redox reaction states in batteries. United States: N. p., 2020. Web. doi:10.1039/d0dt01782e.
Wu, Jue, Yang, Yong, & Yang, Wanli. Advances in soft X-ray RIXS for studying redox reaction states in batteries. United States. https://doi.org/10.1039/d0dt01782e
Wu, Jue, Yang, Yong, and Yang, Wanli. Fri . "Advances in soft X-ray RIXS for studying redox reaction states in batteries". United States. https://doi.org/10.1039/d0dt01782e. https://www.osti.gov/servlets/purl/1845093.
@article{osti_1845093,
title = {Advances in soft X-ray RIXS for studying redox reaction states in batteries},
author = {Wu, Jue and Yang, Yong and Yang, Wanli},
abstractNote = {Redox (reduction and oxidation) chemistry provides the fundamental basis for numerous energy-related electrochemical devices. Detecting the electrochemical redox chemistry is pivotal but challenging because it requires independent probes of the cationic and anionic redox states at different electrochemical states. Here, the synchrotron-based soft X-ray mapping of resonant inelastic X-ray scattering (mRIXS) has recently emerged as a powerful tool for exploring such states in electrochemical devices, especially batteries. High-efficiency mRIXS covers the energy range of the absorption edge with the extra dimension of information on the emitted photon energies. In this frontier article, we review recent representative demonstrations of utilizing soft X-ray mRIXS for detecting the novel chemical state during electrochemical operation and for quantifying the cationic redox reactions through inverse partial fluorescence yield analysis (mRIXS-iPFY). More importantly, the non-divalent states of oxygen in electrodes involving oxygen redox reactions could be reliably captured by mRIXS, with its reversibility quantified by the intensity variation of the characteristic mRIXS feature through a super-partial fluorescence yield analysis (mRIXS-sPFY). These recent demonstrations inspire future perspectives on using mRIXS for studying the complex phenomena in energy materials, with both technical and scientific challenges in RIXS theory, in situ/operando experiments, and spatially resolved RIXS imaging.},
doi = {10.1039/d0dt01782e},
journal = {Dalton Transactions},
number = 39,
volume = 49,
place = {United States},
year = {Fri Jul 17 00:00:00 EDT 2020},
month = {Fri Jul 17 00:00:00 EDT 2020}
}

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