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Title: Elucidating anionic oxygen activity in lithium-rich layered oxides

Abstract

Recent research has explored combining conventional transition metal redox with anionic lattice oxygen redox as a new and exciting direction to search for high-capacity lithium-ion cathodes. For this study, we probe the poorly understood electrochemical activity of anionic oxygen from a material perspective by elucidating the effect of the transition metal on oxygen redox activity. We study two lithium-rich layered oxides, specifically lithium nickel metal oxides where metal is either manganese or ruthenium, which possess similar structure and discharge characteristics, but exhibit distinctly different charge profiles. By combining X-ray spectroscopy with operando differential electrochemical mass spectrometry, we reveal completely different oxygen redox activity in each material, likely resulting from the different interaction between the lattice oxygen and transition metals. This work provides additional insights into the complex mechanism of oxygen redox and development of advanced high-capacity lithium-ion cathodes.

Authors:
 [1];  [1];  [2];  [3];  [4];  [4];  [5]; ORCiD logo [6]; ORCiD logo [5];  [7]; ORCiD logo [7];  [8]; ORCiD logo [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  4. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Sciences Division
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOD National Defense Science and Engineering Graduate Fellowship (NDSEG); U.S. Department of Defense (DOD)
OSTI Identifier:
1433135
Alternate Identifier(s):
OSTI ID: 1430859; OSTI ID: 1461334
Report Number(s):
BNL-203383-2018-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704; AC02-05CH11231; AC02-76SF00515; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Lithium ion battery; cathode; Li-rich; oxygen; batteries; electrochemistry

Citation Formats

Xu, Jing, Sun, Meiling, Qiao, Ruimin, Renfrew, Sara E., Ma, Lu, Wu, Tianpin, Hwang, Sooyeon, Nordlund, Dennis, Su, Dong, Amine, Khalil, Lu, Jun, McCloskey, Bryan D., Yang, Wanli, and Tong, Wei. Elucidating anionic oxygen activity in lithium-rich layered oxides. United States: N. p., 2018. Web. doi:10.1038/s41467-018-03403-9.
Xu, Jing, Sun, Meiling, Qiao, Ruimin, Renfrew, Sara E., Ma, Lu, Wu, Tianpin, Hwang, Sooyeon, Nordlund, Dennis, Su, Dong, Amine, Khalil, Lu, Jun, McCloskey, Bryan D., Yang, Wanli, & Tong, Wei. Elucidating anionic oxygen activity in lithium-rich layered oxides. United States. doi:10.1038/s41467-018-03403-9.
Xu, Jing, Sun, Meiling, Qiao, Ruimin, Renfrew, Sara E., Ma, Lu, Wu, Tianpin, Hwang, Sooyeon, Nordlund, Dennis, Su, Dong, Amine, Khalil, Lu, Jun, McCloskey, Bryan D., Yang, Wanli, and Tong, Wei. Mon . "Elucidating anionic oxygen activity in lithium-rich layered oxides". United States. doi:10.1038/s41467-018-03403-9. https://www.osti.gov/servlets/purl/1433135.
@article{osti_1433135,
title = {Elucidating anionic oxygen activity in lithium-rich layered oxides},
author = {Xu, Jing and Sun, Meiling and Qiao, Ruimin and Renfrew, Sara E. and Ma, Lu and Wu, Tianpin and Hwang, Sooyeon and Nordlund, Dennis and Su, Dong and Amine, Khalil and Lu, Jun and McCloskey, Bryan D. and Yang, Wanli and Tong, Wei},
abstractNote = {Recent research has explored combining conventional transition metal redox with anionic lattice oxygen redox as a new and exciting direction to search for high-capacity lithium-ion cathodes. For this study, we probe the poorly understood electrochemical activity of anionic oxygen from a material perspective by elucidating the effect of the transition metal on oxygen redox activity. We study two lithium-rich layered oxides, specifically lithium nickel metal oxides where metal is either manganese or ruthenium, which possess similar structure and discharge characteristics, but exhibit distinctly different charge profiles. By combining X-ray spectroscopy with operando differential electrochemical mass spectrometry, we reveal completely different oxygen redox activity in each material, likely resulting from the different interaction between the lattice oxygen and transition metals. This work provides additional insights into the complex mechanism of oxygen redox and development of advanced high-capacity lithium-ion cathodes.},
doi = {10.1038/s41467-018-03403-9},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Mon Mar 05 00:00:00 EST 2018},
month = {Mon Mar 05 00:00:00 EST 2018}
}

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Works referenced in this record:

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