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Title: Reversible Anionic Redox Activities in Conventional LiNi1/3Co1/3Mn1/3O2 Cathodes

Abstract

Redox reactions of oxygen have been considered critical in controlling the electrochemical properties of lithium-excessive layered-oxide electrodes. However, conventional electrode materials without overlithiation remain the most practical. Typically, cationic redox reactions are believed to dominate the electrochemical processes in conventional electrodes. Herein, we show unambiguous evidence of reversible anionic redox reactions in LiNi1/3Co1/3Mn1/3O2. The typical involvement of oxygen through hybridization with transition metals is discussed, as well as the intrinsic oxygen redox process at high potentials, which is 75 % reversible during initial cycling and 63% retained after 10 cycles. Our results clarify the reaction mechanism at high potentials in conventional layered electrodes involving both cationic and anionic reactions and indicate the potential of utilizing reversible oxygen redox reactions in conventional layered oxides for high-capacity lithium-ion batteries.

Authors:
 [1];  [2];  [3];  [4];  [5];  [2];  [6]
  1. Dongguk University, Department of Energy and Materials Engineering, KOREA, REPUBLIC OF
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Kyung Hee Univ.-Global Campus, Yongin (Korea). Dept. of Mechanical Engineering
  4. Univ. of Texas at Dallas, Richardson, TX (United States). Dept. of Materials Science and Engineering
  5. Seoul National Univ. (Korea). Inst. of Advanced Machines and Design
  6. Dongguk Univ., Seoul (Korea). Dept. of Energy and Materials Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Research Foundation of Korea (NRF)
OSTI Identifier:
1601226
Alternate Identifier(s):
OSTI ID: 1606068
Grant/Contract Number:  
AC02-05CH11231; 2012R1A3A2048841; 2017R1A2B3004383
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 22; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electrochemistry; Mapping of resonant inelastic X-ray scattering (mRIXS); Lithium ion batteries; Redox chemistry; X-ray absorption spectroscopy

Citation Formats

Lee, Gi-Hyeok, Wu, Jinpeng, Kim, Duho, Cho, Kyeongjae, Cho, Maenghyo, Yang, Wanli, and Kang, Y. M. Reversible Anionic Redox Activities in Conventional LiNi1/3Co1/3Mn1/3O2 Cathodes. United States: N. p., 2020. Web. https://doi.org/10.1002/anie.202001349.
Lee, Gi-Hyeok, Wu, Jinpeng, Kim, Duho, Cho, Kyeongjae, Cho, Maenghyo, Yang, Wanli, & Kang, Y. M. Reversible Anionic Redox Activities in Conventional LiNi1/3Co1/3Mn1/3O2 Cathodes. United States. https://doi.org/10.1002/anie.202001349
Lee, Gi-Hyeok, Wu, Jinpeng, Kim, Duho, Cho, Kyeongjae, Cho, Maenghyo, Yang, Wanli, and Kang, Y. M. Fri . "Reversible Anionic Redox Activities in Conventional LiNi1/3Co1/3Mn1/3O2 Cathodes". United States. https://doi.org/10.1002/anie.202001349. https://www.osti.gov/servlets/purl/1601226.
@article{osti_1601226,
title = {Reversible Anionic Redox Activities in Conventional LiNi1/3Co1/3Mn1/3O2 Cathodes},
author = {Lee, Gi-Hyeok and Wu, Jinpeng and Kim, Duho and Cho, Kyeongjae and Cho, Maenghyo and Yang, Wanli and Kang, Y. M.},
abstractNote = {Redox reactions of oxygen have been considered critical in controlling the electrochemical properties of lithium-excessive layered-oxide electrodes. However, conventional electrode materials without overlithiation remain the most practical. Typically, cationic redox reactions are believed to dominate the electrochemical processes in conventional electrodes. Herein, we show unambiguous evidence of reversible anionic redox reactions in LiNi1/3Co1/3Mn1/3O2. The typical involvement of oxygen through hybridization with transition metals is discussed, as well as the intrinsic oxygen redox process at high potentials, which is 75 % reversible during initial cycling and 63% retained after 10 cycles. Our results clarify the reaction mechanism at high potentials in conventional layered electrodes involving both cationic and anionic reactions and indicate the potential of utilizing reversible oxygen redox reactions in conventional layered oxides for high-capacity lithium-ion batteries.},
doi = {10.1002/anie.202001349},
journal = {Angewandte Chemie (International Edition)},
number = 22,
volume = 59,
place = {United States},
year = {2020},
month = {2}
}

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Cited by: 6 works
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