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Title: Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials

Abstract

There is an urgent need for low-cost, resource-friendly, high-energy-density cathode materials for lithium-ion batteries to satisfy the rapidly increasing need for electrical energy storage. To replace the nickel and cobalt, which are limited resources and are associated with safety problems, in current lithium-ion batteries, high-capacity cathodes based on manganese would be particularly desirable owing to the low cost and high abundance of the metal, and the intrinsic stability of the Mn4+ oxidation state. Here we present a strategy of combining high-valent cations and the partial substitution of fluorine for oxygen in a disordered-rocksalt structure to incorporate the reversible Mn2+/Mn4+ double redox couple into lithium-excess cathode materials. The lithium-rich cathodes thus produced have high capacity and energy density. The use of the Mn2+/Mn4+ redox reduces oxygen redox activity, thereby stabilizing the materials, and opens up new opportunities for the design of high-performance manganese-rich cathodes for advanced lithium-ion batteries.

Authors:
 [1];  [2];  [1];  [3];  [4];  [5];  [1];  [1];  [1];  [6];  [7];  [3];  [8]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  3. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division. Advanced Photon Source
  4. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  6. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source; Univ. of California, Santa Cruz, CA (United States). Dept. of Chemistry and Biochemistry
  8. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1461423
Alternate Identifier(s):
OSTI ID: 1530348
Grant/Contract Number:  
AC02-06CH11357; AC02-05CH11231; ACI-1548562; DGE-1106400; DMR-1720256
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 556; Journal Issue: 7700; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; atomistic models; batteries

Citation Formats

Lee, Jinhyuk, Kitchaev, Daniil A., Kwon, Deok-Hwang, Lee, Chang-Wook, Papp, Joseph K., Liu, Yi-Sheng, Lun, Zhengyan, Clement, Raphaele J., Shi, Tan, McCloskey, Bryan D., Guo, Jinghua, Balasubramanian, Mahalingam, and Ceder, Gerbrand. Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials. United States: N. p., 2018. Web. doi:10.1038/s41586-018-0015-4.
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Lee, Jinhyuk, Kitchaev, Daniil A., Kwon, Deok-Hwang, Lee, Chang-Wook, Papp, Joseph K., Liu, Yi-Sheng, Lun, Zhengyan, Clement, Raphaele J., Shi, Tan, McCloskey, Bryan D., Guo, Jinghua, Balasubramanian, Mahalingam, & Ceder, Gerbrand. Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials. United States. https://doi.org/10.1038/s41586-018-0015-4
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Lee, Jinhyuk, Kitchaev, Daniil A., Kwon, Deok-Hwang, Lee, Chang-Wook, Papp, Joseph K., Liu, Yi-Sheng, Lun, Zhengyan, Clement, Raphaele J., Shi, Tan, McCloskey, Bryan D., Guo, Jinghua, Balasubramanian, Mahalingam, and Ceder, Gerbrand. Wed . "Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials". United States. https://doi.org/10.1038/s41586-018-0015-4. https://www.osti.gov/servlets/purl/1461423.
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@article{osti_1461423,
title = {Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials},
author = {Lee, Jinhyuk and Kitchaev, Daniil A. and Kwon, Deok-Hwang and Lee, Chang-Wook and Papp, Joseph K. and Liu, Yi-Sheng and Lun, Zhengyan and Clement, Raphaele J. and Shi, Tan and McCloskey, Bryan D. and Guo, Jinghua and Balasubramanian, Mahalingam and Ceder, Gerbrand},
abstractNote = {There is an urgent need for low-cost, resource-friendly, high-energy-density cathode materials for lithium-ion batteries to satisfy the rapidly increasing need for electrical energy storage. To replace the nickel and cobalt, which are limited resources and are associated with safety problems, in current lithium-ion batteries, high-capacity cathodes based on manganese would be particularly desirable owing to the low cost and high abundance of the metal, and the intrinsic stability of the Mn4+ oxidation state. Here we present a strategy of combining high-valent cations and the partial substitution of fluorine for oxygen in a disordered-rocksalt structure to incorporate the reversible Mn2+/Mn4+ double redox couple into lithium-excess cathode materials. The lithium-rich cathodes thus produced have high capacity and energy density. The use of the Mn2+/Mn4+ redox reduces oxygen redox activity, thereby stabilizing the materials, and opens up new opportunities for the design of high-performance manganese-rich cathodes for advanced lithium-ion batteries.},
doi = {10.1038/s41586-018-0015-4},
journal = {Nature (London)},
number = 7700,
volume = 556,
place = {United States},
year = {Wed Apr 11 00:00:00 EDT 2018},
month = {Wed Apr 11 00:00:00 EDT 2018}
}
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https://doi.org/10.1038/s41586-018-0015-4
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    • Feng, Ze; Huang, Xiaobing; Rajagopalan, Ranjusha
    • Journal of The Electrochemical Society, Vol. 166, Issue 8
    • DOI: 10.1149/2.0331908jes

    Ultrathin Al2O3 Coating on LiNi0.8Co0.1Mn0.1O2 Cathode Material for Enhanced Cycleability at Extended Voltage Ranges
    journal, February 2019

    Scavenging Materials to Stabilize LiPF 6 ‐Containing Carbonate‐Based Electrolytes for Li‐Ion Batteries
    journal, November 2018

    Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies
    journal, December 2019

    • Liang, Longwei; Zhang, Wenheng; Zhao, Fei
    • Advanced Materials Interfaces, Vol. 7, Issue 3
    • DOI: 10.1002/admi.201901749

    Ethylene Carbonate‐Free Electrolytes for High‐Nickel Layered Oxide Cathodes in Lithium‐Ion Batteries
    journal, June 2019

    • Li, Wangda; Dolocan, Andrei; Li, Jianyu
    • Advanced Energy Materials, Vol. 9, Issue 29
    • DOI: 10.1002/aenm.201901152

    Li 2 O:Li–Mn–O Disordered Rock‐Salt Nanocomposites as Cathode Prelithiation Additives for High‐Energy Density Li‐Ion Batteries
    journal, January 2020

    • Diaz‐Lopez, Maria; Chater, Philip A.; Bordet, Pierre
    • Advanced Energy Materials, Vol. 10, Issue 7
    • DOI: 10.1002/aenm.201902788

    Effect of Fluorination on Lithium Transport and Short‐Range Order in Disordered‐Rocksalt‐Type Lithium‐Ion Battery Cathodes
    journal, March 2020

    • Ouyang, Bin; Artrith, Nongnuch; Lun, Zhengyan
    • Advanced Energy Materials, Vol. 10, Issue 10
    • DOI: 10.1002/aenm.201903240

    Hin und zurück – die Entwicklung von LiNiO 2 als Kathodenaktivmaterial
    journal, May 2019

    • Bianchini, Matteo; Roca‐Ayats, Maria; Hartmann, Pascal
    • Angewandte Chemie, Vol. 131, Issue 31
    • DOI: 10.1002/ange.201812472

    Kathodenmaterialien für wiederaufladbare Lithiumbatterien
    journal, November 2019

    • Lee, Wontae; Muhammad, Shoaib; Sergey, Chernov
    • Angewandte Chemie, Vol. 132, Issue 7
    • DOI: 10.1002/ange.201902359

    Volatility drivers on the metal market and exposure of producing countries
    journal, August 2019

    Electrochemical surface passivation of LiCoO2 particles at ultrahigh voltage and its applications in lithium-based batteries
    journal, November 2018

    High-rate capability and long-term cycling of self-assembled hierarchical Fe 3 O 4 /carbon hollow spheres through interfacial control
    journal, January 2019

    • Huang, Jing; Cheng, Songpu; Chen, Yuxi
    • Journal of Materials Chemistry A, Vol. 7, Issue 28
    • DOI: 10.1039/c9ta04041b

    Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides.
    text, January 2019

    • Hua, Weibo; Wang, Suning; Knapp, Michael
    • Apollo - University of Cambridge Repository
    • DOI: 10.17863/cam.47412

    Multi-anionic and -cationic compounds: New high entropy materials for advanced Li-ion batteries
    other, January 2019

    • Wang, Qingsong; Sarkar, Abhishek; Wang, Di
    • Cambridge : Royal Society of Chemistry
    • DOI: 10.15488/9843

    Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries
    other, January 2019

    • Wang, Qingsong; Sarkar, Abhishek; Wang, Di
    • Cambridge : RSC
    • DOI: 10.15488/10767

    Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides
    text, January 2019

    • Hua, Weibo; Wang, Suning; Knapp, Michael
    • Apollo - University of Cambridge Repository
    • DOI: 10.17863/cam.60446

    Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides
    text, January 2019

    • Hua, Weibo; Wang, Suning; Knapp, Michael
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-04472
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