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:
-
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division. Advanced Photon Source
- Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
- 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
- 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
- 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.
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
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.
@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}
}
Web of Science
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Non-stoichiometric defect-controlled reduction toward mixed-valence Mn-doped hexaaluminates and their optical applications
journal, January 2019
- Hu, Jieqi; Song, Enhai; Zhou, Yayun
- Journal of Materials Chemistry C, Vol. 7, Issue 19
Electrochemical trapping of metastable Mn 3+ ions for activation of MnO 2 oxygen evolution catalysts
journal, May 2018
- Morgan Chan, Zamyla; Kitchaev, Daniil A.; Nelson Weker, Johanna
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 23
Enhanced Electrochemical Properties of LiNi 0.8 Co 0.1 Mn 0.1 O 2 at Elevated Temperature by Simultaneous Structure and Interface Regulating
journal, January 2019
- Feng, Ze; Huang, Xiaobing; Rajagopalan, Ranjusha
- Journal of The Electrochemical Society, Vol. 166, Issue 8
Synthesis and Electrochemical Performance of ZnSe Electrospinning Nanofibers as an Anode Material for Lithium Ion and Sodium Ion Batteries
journal, August 2019
- Zhou, Peng; Zhang, Mingyu; Wang, Liping
- Frontiers in Chemistry, Vol. 7
Ultrathin Al2O3 Coating on LiNi0.8Co0.1Mn0.1O2 Cathode Material for Enhanced Cycleability at Extended Voltage Ranges
journal, February 2019
- Zhu, Wenchang; Huang, Xue; Liu, Tingting
- Coatings, Vol. 9, Issue 2
Scavenging Materials to Stabilize LiPF 6 ‐Containing Carbonate‐Based Electrolytes for Li‐Ion Batteries
journal, November 2018
- Han, Jung‐Gu; Kim, Koeun; Lee, Yongwon
- Advanced Materials, Vol. 31, Issue 20
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
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
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
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
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
Kathodenmaterialien für wiederaufladbare Lithiumbatterien
journal, November 2019
- Lee, Wontae; Muhammad, Shoaib; Sergey, Chernov
- Angewandte Chemie, Vol. 132, Issue 7
Volatility drivers on the metal market and exposure of producing countries
journal, August 2019
- Renner, Sven; Wellmer, Friedrich W.
- Mineral Economics, Vol. 33, Issue 3
Electrochemical surface passivation of LiCoO2 particles at ultrahigh voltage and its applications in lithium-based batteries
journal, November 2018
- Qian, Jiawei; Liu, Lei; Yang, Jixiang
- Nature Communications, Vol. 9, Issue 1
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
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
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
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
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
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
Improved cycling stability in high-capacity Li-rich vanadium containing disordered rock salt oxyfluoride cathodes
text, January 2019
- Baur, C.; Källquist, I.; Chable, J.
- Karlsruhe