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

Lee, Gi-Hyeok; Wu, Jinpeng; Kim, Duho; Cho, Kyeongjae; Cho, Maenghyo; Yang, Wanli; Kang, Y. M.

doi:10.1002/anie.202001349

Title: Reversible Anionic Redox Activities in Conventional LiNi_1/3Co_1/3Mn_1/3O₂ Cathodes

Journal Article · 07 February 2020 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202001349 · OSTI ID:1601226

Lee, Gi-Hyeok ^[1]; Wu, Jinpeng ^[2]; Kim, Duho ^[3]; Cho, Kyeongjae ^[4]; Cho, Maenghyo ^[5]; Yang, Wanli ^[2]; Kang, Y. M. ^[6]

Dongguk University, Department of Energy and Materials Engineering, KOREA, REPUBLIC OF
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Kyung Hee Univ.-Global Campus, Yongin (Korea). Dept. of Mechanical Engineering
Univ. of Texas at Dallas, Richardson, TX (United States). Dept. of Materials Science and Engineering
Seoul National Univ. (Korea). Inst. of Advanced Machines and Design
Dongguk Univ., Seoul (Korea). Dept. of Energy and Materials Engineering

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 LiNi_1/3Co_1/3Mn_1/3O₂. 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Research Foundation of Korea (NRF)

Grant/Contract Number:: AC02-05CH11231; 2012R1A3A2048841; 2017R1A2B3004383

OSTI ID:: 1601226

Alternate ID(s):: OSTI ID: 1606068

Journal Information:: Angewandte Chemie (International Edition), Vol. 59, Issue 22; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 83 works

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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

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

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Title: Reversible Anionic Redox Activities in Conventional LiNi_1/3Co_1/3Mn_1/3O₂ Cathodes