DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: A reflection on lithium-ion battery cathode chemistry

Abstract

Abstract Lithium-ion batteries have aided the portable electronics revolution for nearly three decades. They are now enabling vehicle electrification and beginning to enter the utility industry. The emergence and dominance of lithium-ion batteries are due to their higher energy density compared to other rechargeable battery systems, enabled by the design and development of high-energy density electrode materials. Basic science research, involving solid-state chemistry and physics, has been at the center of this endeavor, particularly during the 1970s and 1980s. With the award of the 2019 Nobel Prize in Chemistry to the development of lithium-ion batteries, it is enlightening to look back at the evolution of the cathode chemistry that made the modern lithium-ion technology feasible. This review article provides a reflection on how fundamental studies have facilitated the discovery, optimization, and rational design of three major categories of oxide cathodes for lithium-ion batteries, and a personal perspective on the future of this important area.

Authors:
ORCiD logo
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1619620
Alternate Identifier(s):
OSTI ID: 1624263
Grant/Contract Number:  
SC0005397; F-1254
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
Science & Technology - Other Topics

Citation Formats

Manthiram, Arumugam. A reflection on lithium-ion battery cathode chemistry. United Kingdom: N. p., 2020. Web. doi:10.1038/s41467-020-15355-0.
Manthiram, Arumugam. A reflection on lithium-ion battery cathode chemistry. United Kingdom. https://doi.org/10.1038/s41467-020-15355-0
Manthiram, Arumugam. Wed . "A reflection on lithium-ion battery cathode chemistry". United Kingdom. https://doi.org/10.1038/s41467-020-15355-0.
@article{osti_1619620,
title = {A reflection on lithium-ion battery cathode chemistry},
author = {Manthiram, Arumugam},
abstractNote = {Abstract Lithium-ion batteries have aided the portable electronics revolution for nearly three decades. They are now enabling vehicle electrification and beginning to enter the utility industry. The emergence and dominance of lithium-ion batteries are due to their higher energy density compared to other rechargeable battery systems, enabled by the design and development of high-energy density electrode materials. Basic science research, involving solid-state chemistry and physics, has been at the center of this endeavor, particularly during the 1970s and 1980s. With the award of the 2019 Nobel Prize in Chemistry to the development of lithium-ion batteries, it is enlightening to look back at the evolution of the cathode chemistry that made the modern lithium-ion technology feasible. This review article provides a reflection on how fundamental studies have facilitated the discovery, optimization, and rational design of three major categories of oxide cathodes for lithium-ion batteries, and a personal perspective on the future of this important area.},
doi = {10.1038/s41467-020-15355-0},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {Wed Mar 25 00:00:00 EDT 2020},
month = {Wed Mar 25 00:00:00 EDT 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-020-15355-0

Citation Metrics:
Cited by: 1002 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Positions of the redox energies relative to the top of the anion: p bands. The top of the S2−:3p band lying at a higher energy limits the cell voltage to <2.5 V with a sulfide cathode. In contrast, the top of the O2−:2p band lying at a lowermore » energy enables access to lower-lying energy bands with higher oxidation states and increases the cell voltage substantially to ~4 V.« less

Save / Share:

Works referenced in this record:

Electron-Electron Scattering in Ti S 2
journal, December 1975


Improved capacity retention in rechargeable 4 V lithium/lithium-manganese oxide (spinel) cells
journal, April 1994


Current Status and Future Prospects of Metal–Sulfur Batteries
journal, May 2019


Lithium insertion into Fe2(MO4)3 frameworks: Comparison of M = W with M = Mo
journal, December 1987


Lattice doping regulated interfacial reactions in cathode for enhanced cycling stability
journal, August 2019


Structural characterization of the lithiated iron oxides LixFe3O4 and LixFe2O3 (0<x<2)
journal, June 1982


Demonstrating Oxygen Loss and Associated Structural Reorganization in the Lithium Battery Cathode Li[Ni0.2Li0.2Mn0.6]O2
journal, June 2006

  • Armstrong, A. Robert; Holzapfel, Michael; Novák, Petr
  • Journal of the American Chemical Society, Vol. 128, Issue 26
  • DOI: 10.1021/ja062027+

Mn(II) deposition on anodes and its effects on capacity fade in spinel lithium manganate–carbon systems
journal, September 2013

  • Zhan, Chun; Lu, Jun; Jeremy Kropf, A.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3437

Thermodynamic Properties of the Potassium–Graphite Lamellar Compounds from Solid‐State emf Measurements
journal, July 1968

  • Aronson, S.; Salzano, F. J.; Bellafiore, D.
  • The Journal of Chemical Physics, Vol. 49, Issue 1
  • DOI: 10.1063/1.1669840

Status of the secondary lithium electrode
journal, January 1981


The electrochemical insertion properties of sodium vanadium fluorophosphate, Na3V2(PO4)2F3
journal, July 2006


Synthesis and structural characterization of the normal spinel Li[Ni2]O4
journal, October 1985


Soft Chemistry Synthesis and Characterization of Layered Li1-xNi1-yCoyO2-δ (0 ≤ x ≤ 1 and 0 ≤ y ≤ 1)
journal, September 2001

  • Chebiam, R. V.; Prado, F.; Manthiram, A.
  • Chemistry of Materials, Vol. 13, Issue 9, p. 2951-2957
  • DOI: 10.1021/cm0102537

Intercalation Complexes of Lewis Bases and Layered Sulfides: A Large Class of New Superconductors
journal, October 1971


Synthesis and Electrochemical Properties of LiCo[sub 2]O[sub 4] Spinel Cathodes
journal, January 2002

  • Choi, S.; Manthiram, A.
  • Journal of The Electrochemical Society, Vol. 149, Issue 2
  • DOI: 10.1149/1.1431574

High-nickel layered oxide cathodes for lithium-based automotive batteries
journal, January 2020


The influence of oxygen variation on the crystal structure and phase composition of the superconductor yttrium barium copper oxide (YBa2Cu3O7-x)
journal, October 1987

  • Manthiram, A.; Swinnea, J. S.; Sui, Z. T.
  • Journal of the American Chemical Society, Vol. 109, Issue 22
  • DOI: 10.1021/ja00256a019

Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011


Li-ion battery materials: present and future
journal, June 2015


Low-Temperature Synthesis, Structural Characterization, and Electrochemistry of Ni-Rich Spinel-like LiNi 2– y Mn y O 4 (0.4 ≤ y ≤ 1)
journal, November 2015


Structural Considerations of Layered and Spinel Lithiated Oxides for Lithium Ion Batteries
journal, January 1995

  • Thackeray, M. M.
  • Journal of The Electrochemical Society, Vol. 142, Issue 8
  • DOI: 10.1149/1.2050053

Synthesis of layered LiMnO2 as an electrode for rechargeable lithium batteries
journal, June 1996

  • Armstrong, A. Robert; Bruce, Peter G.
  • Nature, Vol. 381, Issue 6582
  • DOI: 10.1038/381499a0

Phase Relationships and Structural and Chemical Stabilities of Charged Li[sub 1−x]CoO[sub 2−δ] and Li[sub 1−x]Ni[sub 0.85]Co[sub 0.15]O[sub 2−δ] Cathodes
journal, January 2003

  • Venkatraman, S.; Shin, Y.; Manthiram, A.
  • Electrochemical and Solid-State Letters, Vol. 6, Issue 1
  • DOI: 10.1149/1.1525430

Chemical synthesis and properties of Li1−δ−xNi1+δO2 and Li[Ni2]O4
journal, January 1992


The Li-Ion Rechargeable Battery: A Perspective
journal, January 2013

  • Goodenough, John B.; Park, Kyu-Sung
  • Journal of the American Chemical Society, Vol. 135, Issue 4
  • DOI: 10.1021/ja3091438

Phospho-olivines as Positive-Electrode Materials for Rechargeable Lithium Batteries
journal, April 1997

  • Padhi, A. K.
  • Journal of The Electrochemical Society, Vol. 144, Issue 4, p. 1188-1194
  • DOI: 10.1149/1.1837571

Lithium insertion into Fe2(SO4)3 frameworks
journal, May 1989


Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability
journal, February 2018

  • Li, Wangda; Liu, Xiaoming; Celio, Hugo
  • Advanced Energy Materials, Vol. 8, Issue 15
  • DOI: 10.1002/aenm.201703154

Electrochemical and Structural Properties of xLi2M‘O3 ·(1− x )LiMn0.5Ni0.5O2 Electrodes for Lithium Batteries (M‘ = Ti, Mn, Zr; 0 ≤ x ⩽ 0.3)
journal, May 2004

  • Kim, Jeom-Soo; Johnson, Christopher S.; Vaughey, John T.
  • Chemistry of Materials, Vol. 16, Issue 10, p. 1996-2006
  • DOI: 10.1021/cm0306461

Polyanionic (Phosphates, Silicates, Sulfates) Frameworks as Electrode Materials for Rechargeable Li (or Na) Batteries
journal, June 2013

  • Masquelier, Christian; Croguennec, Laurence
  • Chemical Reviews, Vol. 113, Issue 8
  • DOI: 10.1021/cr3001862

Irreversible conductivity change of Li1−xCoO2 on electrochemical lithium insertion/extraction, desirable for battery applications
journal, January 1998

  • Nishizawa, Matsuhiko; Yamamura, Satoru
  • Chemical Communications, Issue 16
  • DOI: 10.1039/a802962h

A perspective on the high-voltage LiMn1.5Ni0.5O4 spinel cathode for lithium-ion batteries
journal, January 2014

  • Manthiram, Arumugam; Chemelewski, Katharine; Lee, Eun-Sung
  • Energy & Environmental Science, Vol. 7, Issue 4
  • DOI: 10.1039/c3ee42981d

An Outlook on Lithium Ion Battery Technology
journal, September 2017


Metallic oxides
journal, January 1971


Comparison of Metal Ion Dissolutions from Lithium Ion Battery Cathodes
journal, January 2006

  • Choi, W.; Manthiram, A.
  • Journal of The Electrochemical Society, Vol. 153, Issue 9
  • DOI: 10.1149/1.2219710

Carbon coated Na3V2(PO4)3 as novel electrode material for sodium ion batteries
journal, January 2012


Lithium-Sulfur Batteries: Attaining the Critical Metrics
journal, February 2020


Electrical Energy Storage and Intercalation Chemistry
journal, June 1976


Comparison of the chemical stability of the high energy density cathodes of lithium-ion batteries
journal, November 2001


Lithium insertion into manganese spinels
journal, April 1983

  • Thackeray, M. M.; David, W. I. F.; Bruce, P. G.
  • Materials Research Bulletin, Vol. 18, Issue 4, p. 461-472
  • DOI: 10.1016/0025-5408(83)90138-1

Modified High-Nickel Cathodes with Stable Surface Chemistry Against Ambient Air for Lithium-Ion Batteries
journal, April 2018

  • You, Ya; Celio, Hugo; Li, Jianyu
  • Angewandte Chemie International Edition, Vol. 57, Issue 22
  • DOI: 10.1002/anie.201801533

Fundamental understanding and practical challenges of anionic redox activity in Li-ion batteries
journal, April 2018


Topochemically controlled hydrogen reduction of scheelite-related rare-earth metal molybdates
journal, January 1981

  • Gopalakrishnan, Jagannatha; Manthiram, Arumugam
  • Journal of the Chemical Society, Dalton Transactions, Issue 3
  • DOI: 10.1039/dt9810000668

Building better batteries
journal, February 2008

  • Armand, M.; Tarascon, J.-M.
  • Nature, Vol. 451, Issue 7179, p. 652-657
  • DOI: 10.1038/451652a

Synthesis and Electrochemistry of LiNi[sub x]Mn[sub 2−x]O[sub 4]
journal, January 1997

  • Zhong, Qiming
  • Journal of The Electrochemical Society, Vol. 144, Issue 1
  • DOI: 10.1149/1.1837386

Structural characterization of delithiated LiVO2
journal, November 1984


Historical development of secondary lithium batteries
journal, August 1994


Insertion/extraction reactions of lithium with LiV2O4
journal, December 1985


Li–O2 and Li–S batteries with high energy storage
journal, January 2012

  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191

Preparation of a new crystal form of manganese dioxide: λ-MnO2
journal, September 1981


Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries
journal, April 2017

  • Li, Wangda; Dolocan, Andrei; Oh, Pilgun
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14589

A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries
journal, May 2009

  • Ji, Xiulei; Lee, Kyu Tae; Nazar, Linda F.
  • Nature Materials, Vol. 8, Issue 6, p. 500-506
  • DOI: 10.1038/nmat2460

LixCoO2 (0<x<-1): A new cathode material for batteries of high energy density
journal, June 1980


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.