Ethylene Carbonate–Free Electrolytes for High–Nickel Layered Oxide Cathodes in Lithium–Ion Batteries
Abstract
Abstract Layered lithium nickel oxide (LiNiO 2 ) can provide very high energy density among intercalation cathode materials for lithium‐ion batteries, but suffers from poor cycle life and thermal‐abuse tolerance with large lithium utilization. In addition to stabilization of the active cathode material, a concurrent development of electrolyte systems of better compatibility is critical to overcome these limitations for practical applications. Here, with nonaqueous electrolytes based on exclusively aprotic acyclic carbonates free of ethylene carbonate (EC), superior electrochemical and thermal characteristics are obtained with an ultrahigh‐nickel cathode (LiNi 0.94 Co 0.06 O 2 ), capable of reaching a 235 mA h g −1 specific capacity. Pouch‐type graphite|LiNi 0.94 Co 0.06 O 2 cells in EC‐free electrolytes withstand several hundred charge–discharge cycles with minor degradation at both ambient and elevated temperatures. In thermal‐abuse tests, the cathode at full charge, while reacting aggressively with EC‐based electrolytes below 200 °C, shows suppressed self‐heating without EC. Through 3D chemical and structural analyses, the intriguing impact of EC is visualized in aggravating unwanted surface parasitic reactions and irreversible bulk structural degradation of the cathode at high voltages. These results provide important insights in designing high‐energy electrodes for long‐lasting and reliable lithium‐ion batteries.
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); Welch Foundation; USDOE
- OSTI Identifier:
- 2217332
- Alternate Identifier(s):
- OSTI ID: 1529430
- Grant/Contract Number:
- EE0007762; F-1254; DE‐EE0007762
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 29; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; batteries; cathodes; ethylene carbonate-free electrolytes; high-nickel layered oxide cathodes; in situ X-ray diffraction; lithium-ion batteries; secondary-ion mass spectrometry
Citation Formats
Li, Wangda, Dolocan, Andrei, Li, Jianyu, Xie, Qiang, and Manthiram, Arumugam. Ethylene Carbonate–Free Electrolytes for High–Nickel Layered Oxide Cathodes in Lithium–Ion Batteries. United States: N. p., 2019.
Web. doi:10.1002/aenm.201901152.
Li, Wangda, Dolocan, Andrei, Li, Jianyu, Xie, Qiang, & Manthiram, Arumugam. Ethylene Carbonate–Free Electrolytes for High–Nickel Layered Oxide Cathodes in Lithium–Ion Batteries. United States. https://doi.org/10.1002/aenm.201901152
Li, Wangda, Dolocan, Andrei, Li, Jianyu, Xie, Qiang, and Manthiram, Arumugam. Tue .
"Ethylene Carbonate–Free Electrolytes for High–Nickel Layered Oxide Cathodes in Lithium–Ion Batteries". United States. https://doi.org/10.1002/aenm.201901152. https://www.osti.gov/servlets/purl/2217332.
@article{osti_2217332,
title = {Ethylene Carbonate–Free Electrolytes for High–Nickel Layered Oxide Cathodes in Lithium–Ion Batteries},
author = {Li, Wangda and Dolocan, Andrei and Li, Jianyu and Xie, Qiang and Manthiram, Arumugam},
abstractNote = {Abstract Layered lithium nickel oxide (LiNiO 2 ) can provide very high energy density among intercalation cathode materials for lithium‐ion batteries, but suffers from poor cycle life and thermal‐abuse tolerance with large lithium utilization. In addition to stabilization of the active cathode material, a concurrent development of electrolyte systems of better compatibility is critical to overcome these limitations for practical applications. Here, with nonaqueous electrolytes based on exclusively aprotic acyclic carbonates free of ethylene carbonate (EC), superior electrochemical and thermal characteristics are obtained with an ultrahigh‐nickel cathode (LiNi 0.94 Co 0.06 O 2 ), capable of reaching a 235 mA h g −1 specific capacity. Pouch‐type graphite|LiNi 0.94 Co 0.06 O 2 cells in EC‐free electrolytes withstand several hundred charge–discharge cycles with minor degradation at both ambient and elevated temperatures. In thermal‐abuse tests, the cathode at full charge, while reacting aggressively with EC‐based electrolytes below 200 °C, shows suppressed self‐heating without EC. Through 3D chemical and structural analyses, the intriguing impact of EC is visualized in aggravating unwanted surface parasitic reactions and irreversible bulk structural degradation of the cathode at high voltages. These results provide important insights in designing high‐energy electrodes for long‐lasting and reliable lithium‐ion batteries.},
doi = {10.1002/aenm.201901152},
journal = {Advanced Energy Materials},
number = 29,
volume = 9,
place = {United States},
year = {Tue Jun 25 00:00:00 EDT 2019},
month = {Tue Jun 25 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 78 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Effects of aluminum on the structural and electrochemical properties of LiNiO2
journal, April 2003
- Guilmard, M.
- Journal of Power Sources, Vol. 115, Issue 2
A Guide to Ethylene Carbonate-Free Electrolyte Making for Li-Ion Cells
journal, November 2016
- Ma, Lin; Glazier, S. L.; Petibon, R.
- Journal of The Electrochemical Society, Vol. 164, Issue 1
Inside Cover: Ultra-Tuning of the Aperture Size in Stiffened ZIF-8_Cm Frameworks with Mixed-Linker Strategy for Enhanced CO 2 /CH 4 Separation (Angew. Chem. Int. Ed. 1/2019)
journal, December 2018
- Hou, Qianqian; Wu, Ying; Zhou, Sheng
- Angewandte Chemie International Edition, Vol. 58, Issue 1
Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials
journal, April 2018
- Lee, Jinhyuk; Kitchaev, Daniil A.; Kwon, Deok-Hwang
- Nature, Vol. 556, Issue 7700
Structural Stability of LiNiO 2 Cycled above 4.2 V
journal, April 2017
- Yoon, Chong S.; Jun, Do-Wook; Myung, Seung-Taek
- ACS Energy Letters, Vol. 2, Issue 5
LixNiO2, a promising cathode for rechargeable lithium batteries
journal, March 1995
- Broussely, M.; Perton, F.; Biensan, P.
- Journal of Power Sources, Vol. 54, Issue 1
Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights
journal, October 2015
- Gauthier, Magali; Carney, Thomas J.; Grimaud, Alexis
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 22
Pushing the limit of layered transition metal oxide cathodes for high-energy density rechargeable Li ion batteries
journal, January 2018
- Kim, U. -H.; Jun, D. -W.; Park, K. -J.
- Energy & Environmental Science, Vol. 11, Issue 5
Characterization and cathode performance of Li1 − xNi1 + xO2 prepared with the excess lithium method
journal, September 1995
- Arai, H.
- Solid State Ionics, Vol. 80, Issue 3-4
Thermally driven mesoscale chemomechanical interplay in Li 0.5 Ni 0.6 Mn 0.2 Co 0.2 O 2 cathode materials
journal, January 2018
- Wei, Chenxi; Zhang, Yan; Lee, Sang-Jun
- Journal of Materials Chemistry A, Vol. 6, Issue 45
Rechargeable LiNiO[sub 2]∕Carbon Cells
journal, January 1991
- Dahn, J. R.
- Journal of The Electrochemical Society, Vol. 138, Issue 8
Gas Evolution during Unwanted Lithium Plating in Li-Ion Cells with EC-Based or EC-Free Electrolytes
journal, January 2016
- Liu, Q. Q.; Xiong, D. J.; Petibon, R.
- Journal of The Electrochemical Society, Vol. 163, Issue 14
Singlet Oxygen Reactivity with Carbonate Solvents Used for Li-Ion Battery Electrolytes
journal, October 2018
- Freiberg, Anna T. S.; Roos, Matthias K.; Wandt, Johannes
- The Journal of Physical Chemistry A, Vol. 122, Issue 45
Thermal Stability of Lithium Nickel Oxide Derivatives. Part I: Li x Ni 1.02 O 2 and Li x Ni 0.89 Al 0.16 O 2 ( x = 0.50 and 0.30)
journal, November 2003
- Guilmard, M.; Croguennec, L.; Denux, D.
- Chemistry of Materials, Vol. 15, Issue 23
The Reaction of Charged Cathodes with Nonaqueous Solvents and Electrolytes: I. Li[sub 0.5]CoO[sub 2]
journal, January 2001
- MacNeil, D. D.; Dahn, J. R.
- Journal of The Electrochemical Society, Vol. 148, Issue 11
Origin of voltage decay in high-capacity layered oxide electrodes
journal, December 2014
- Sathiya, M.; Abakumov, A. M.; Foix, D.
- Nature Materials, Vol. 14, Issue 2
Probing Surface Chemistry Changes Using LiCoO 2 -only Electrodes in Li-Ion Batteries
journal, January 2018
- Gauthier, Magali; Karayaylali, Pinar; Giordano, Livia
- Journal of The Electrochemical Society, Vol. 165, Issue 7
Detailed Studies of a High-Capacity Electrode Material for Rechargeable Batteries, Li 2 MnO 3 −LiCo 1/3 Ni 1/3 Mn 1/3 O 2
journal, March 2011
- Yabuuchi, Naoaki; Yoshii, Kazuhiro; Myung, Seung-Taek
- Journal of the American Chemical Society, Vol. 133, Issue 12
Thermal Stability of the Li(Ni[sub 0.8]Co[sub 0.15]Al[sub 0.05])O[sub 2] Cathode in the Presence of Cell Components
journal, January 2006
- Belharouak, I.; Vissers, D.; Amine, K.
- Journal of The Electrochemical Society, Vol. 153, Issue 11
Structure and electrochemistry of LixMnyNi1−yO2
journal, October 1992
- Rossen, E.; Jones, C.; Dahn, J.
- Solid State Ionics, Vol. 57, Issue 3-4
Electrochemistry and Structural Chemistry of LiNiO[sub 2] (R3m) for 4 Volt Secondary Lithium Cells
journal, January 1993
- Ohzuku, Tsutomu
- Journal of The Electrochemical Society, Vol. 140, Issue 7
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries
journal, October 2004
- Xu, Kang
- Chemical Reviews, Vol. 104, Issue 10, p. 4303-4418
A Systematic Study of Electrolyte Additives in Li[Ni 1/3 Mn 1/3 Co 1/3 ]O 2 (NMC)/Graphite Pouch Cells
journal, January 2014
- Wang, David Yaohui; Xia, Jian; Ma, Lin
- Journal of The Electrochemical Society, Vol. 161, Issue 12
Electrolytes and Interphases in Li-Ion Batteries and Beyond
journal, October 2014
- Xu, Kang
- Chemical Reviews, Vol. 114, Issue 23
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
Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy
journal, October 2016
- Wood, Kevin N.; Kazyak, Eric; Chadwick, Alexander F.
- ACS Central Science, Vol. 2, Issue 11
A Study of the Transport Properties of Ethylene Carbonate-Free Li Electrolytes
journal, January 2018
- Logan, E. R.; Tonita, Erin M.; Gering, K. L.
- Journal of The Electrochemical Society, Vol. 165, Issue 3
Collapse of LiNi 1– x – y Co x Mn y O 2 Lattice at Deep Charge Irrespective of Nickel Content in Lithium-Ion Batteries
journal, March 2019
- Li, Wangda; Asl, Hooman Yaghoobnejad; Xie, Qiang
- Journal of the American Chemical Society, Vol. 141, Issue 13
High-voltage positive electrode materials for lithium-ion batteries
journal, January 2017
- Li, Wangda; Song, Bohang; Manthiram, Arumugam
- Chemical Society Reviews, Vol. 46, Issue 10
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
The Study of Surface Phenomena Related to Electrochemical Lithium Intercalation into Li[sub x]MO[sub y] Host Materials (M = Ni, Mn)
journal, January 2000
- Aurbach, Doron; Gamolsky, Kira; Markovsky, Boris
- Journal of The Electrochemical Society, Vol. 147, Issue 4
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
Separating electronic and ionic conductivity in mix-conducting layered lithium transition-metal oxides
journal, July 2018
- Wang, Shanyu; Yan, Mengyu; Li, Yun
- Journal of Power Sources, Vol. 393
Dynamic formation of a solid-liquid electrolyte interphase and its consequences for hybrid-battery concepts
journal, March 2016
- Busche, Martin R.; Drossel, Thomas; Leichtweiss, Thomas
- Nature Chemistry, Vol. 8, Issue 5
Electrolyte System for High Voltage Li-Ion Cells
journal, January 2016
- Petibon, Remi; Xia, Jian; Ma, Lin
- Journal of The Electrochemical Society, Vol. 163, Issue 13
Thermal stability of LixCoO2, LixNiO2 and λ-MnO2 and consequences for the safety of Li-ion cells
journal, August 1994
- Dahn, J.; Fuller, E.; Obrovac, M.
- Solid State Ionics, Vol. 69, Issue 3-4
Some Physical Properties of Ethylene Carbonate-Free Electrolytes
journal, January 2018
- Xiong, D. J.; Bauer, M.; Ellis, L. D.
- Journal of The Electrochemical Society, Vol. 165, Issue 2
Nickel-rich layered LiNi 1−x M x O 2 (M = Mn, Fe, and Co) electrocatalysts with high oxygen evolution reaction activity
journal, January 2015
- Augustyn, Veronica; Therese, Soosairaj; Turner, Travis C.
- Journal of Materials Chemistry A, Vol. 3, Issue 32
Formation and Inhibition of Metallic Lithium Microstructures in Lithium Batteries Driven by Chemical Crossover
journal, May 2017
- Li, Wangda; Kim, Un-Hyuck; Dolocan, Andrei
- ACS Nano, Vol. 11, Issue 6
Prospect and Reality of Ni-Rich Cathode for Commercialization
journal, November 2017
- Kim, Junhyeok; Lee, Hyomyung; Cha, Hyungyeon
- Advanced Energy Materials, Vol. 8, Issue 6
Lithium bis(fluorosulfonyl)imide (LiFSI) as conducting salt for nonaqueous liquid electrolytes for lithium-ion batteries: Physicochemical and electrochemical properties
journal, April 2011
- Han, Hong-Bo; Zhou, Si-Si; Zhang, Dai-Jun
- Journal of Power Sources, Vol. 196, Issue 7
Fundamental understanding and practical challenges of anionic redox activity in Li-ion batteries
journal, April 2018
- Assat, Gaurav; Tarascon, Jean-Marie
- Nature Energy, Vol. 3, Issue 5
Thermal Reactions Between Delithiated Lithium Nickelate and Electrolyte Solutions
journal, January 2002
- Arai, Hajime; Tsuda, Masayuki; Saito, Keiichi
- Journal of The Electrochemical Society, Vol. 149, Issue 4
High-Performance LiNiO 2 Cathodes with Practical Loading Cycled with Li metal Anodes in Fluoroethylene Carbonate-Based Electrolyte Solution
journal, May 2018
- Markevich, Elena; Salitra, Gregory; Talyosef, Yosef
- ACS Applied Energy Materials, Vol. 1, Issue 6
A highly stabilized nickel-rich cathode material by nanoscale epitaxy control for high-energy lithium-ion batteries
journal, January 2018
- Kim, Junhyeok; Ma, Hyunsoo; Cha, Hyungyeon
- Energy & Environmental Science, Vol. 11, Issue 6
A Mg-Doped High-Nickel Layered Oxide Cathode Enabling Safer, High-Energy-Density Li-Ion Batteries
journal, January 2019
- Xie, Qiang; Li, Wangda; Manthiram, Arumugam
- Chemistry of Materials, Vol. 31, Issue 3
Comparative study of LiCoO2, LiNi12Co12O2 and LiNiO2 for 4 volt secondary lithium cells
journal, June 1993
- Ohzuku, Tsutomu; Ueda, Atsushi; Nagayama, Masatoshi
- Electrochimica Acta, Vol. 38, Issue 9
Effects of Electrolyte Additives and Solvents on Unwanted Lithium Plating in Lithium-Ion Cells
journal, January 2017
- Liu, Q. Q.; Petibon, R.; Du, C. Y.
- Journal of The Electrochemical Society, Vol. 164, Issue 6
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
Interfacial Chemistry in Solid-State Batteries: Formation of Interphase and Its Consequences
journal, December 2017
- Wang, Shaofei; Xu, Henghui; Li, Wangda
- Journal of the American Chemical Society, Vol. 140, Issue 1
The cycling properties of the LixNi1−yCoyO2 electrode
journal, April 1993
- Delmas, C.; Saadoune, I.; Rougier, A.
- Journal of Power Sources, Vol. 44, Issue 1-3