Long-life LiNi0.5Mn1.5O4/graphite lithium-ion cells with an artificial graphite-electrolyte interface
Abstract
The high operating voltage of a spinel LiNi0.5Mn1.5O4 (LNMO) cathode leads to electrolyte decomposition and accelerated deterioration of the electrode/electrolyte interface in lithium-ion cells. Aggressive side reactions prevent long-term cycling and hinder its practical application. Advanced characterization shows that the high-voltage operation makes the graphite anode react with the electrolyte, particularly with the lithium salt in the electrolyte, resulting in massive active lithium inventory loss and capacity fade. The side reactions at the graphite are identified as the main culprit for the LNMO/graphite full cell decay. Here, we demonstrate that an artificial solid-electrolyte interface layer consisting of an ultra-thin Al2O3 film, generated via atomic layer deposition (ALD) at the graphite surface, can successfully isolate the graphite from the electrolyte and inhibit the undesired reactions. Consequently, the capacity and cycling stability of the LNMO/graphite cell are drastically improved. After 300 cycles, the capacity retention of LNMO/graphite cell increases from 57.7% to 98.6% with the ALD-coated graphite. Furthermore, our findings provide valuable insights into the LNMO/graphite cell degradation and suggest a simple and robust, yet highly effective, approach for the practical viability of high-voltage lithium-ion batteries.
- Authors:
-
- Univ. of Texas at Austin, TX (United States)
- Publication Date:
- Research Org.:
- Univ. of Texas at Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1969456
- Alternate Identifier(s):
- OSTI ID: 1825204
- Grant/Contract Number:
- EE0008442
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy Storage Materials
- Additional Journal Information:
- Journal Volume: 43; Journal ID: ISSN 2405-8297
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; High-voltage spinel cathode; Graphite anode; Atomic layer deposition; Secondary-ion mass spectrometry; Degradation mechanisms
Citation Formats
Zou, Feng, Nallan, Himamshu C., Dolocan, Andrei, Xie, Qiang, Li, Jianyu, Coffey, Brennan M., Ekerdt, John G., and Manthiram, Arumugam. Long-life LiNi0.5Mn1.5O4/graphite lithium-ion cells with an artificial graphite-electrolyte interface. United States: N. p., 2021.
Web. doi:10.1016/j.ensm.2021.09.033.
Zou, Feng, Nallan, Himamshu C., Dolocan, Andrei, Xie, Qiang, Li, Jianyu, Coffey, Brennan M., Ekerdt, John G., & Manthiram, Arumugam. Long-life LiNi0.5Mn1.5O4/graphite lithium-ion cells with an artificial graphite-electrolyte interface. United States. https://doi.org/10.1016/j.ensm.2021.09.033
Zou, Feng, Nallan, Himamshu C., Dolocan, Andrei, Xie, Qiang, Li, Jianyu, Coffey, Brennan M., Ekerdt, John G., and Manthiram, Arumugam. Tue .
"Long-life LiNi0.5Mn1.5O4/graphite lithium-ion cells with an artificial graphite-electrolyte interface". United States. https://doi.org/10.1016/j.ensm.2021.09.033. https://www.osti.gov/servlets/purl/1969456.
@article{osti_1969456,
title = {Long-life LiNi0.5Mn1.5O4/graphite lithium-ion cells with an artificial graphite-electrolyte interface},
author = {Zou, Feng and Nallan, Himamshu C. and Dolocan, Andrei and Xie, Qiang and Li, Jianyu and Coffey, Brennan M. and Ekerdt, John G. and Manthiram, Arumugam},
abstractNote = {The high operating voltage of a spinel LiNi0.5Mn1.5O4 (LNMO) cathode leads to electrolyte decomposition and accelerated deterioration of the electrode/electrolyte interface in lithium-ion cells. Aggressive side reactions prevent long-term cycling and hinder its practical application. Advanced characterization shows that the high-voltage operation makes the graphite anode react with the electrolyte, particularly with the lithium salt in the electrolyte, resulting in massive active lithium inventory loss and capacity fade. The side reactions at the graphite are identified as the main culprit for the LNMO/graphite full cell decay. Here, we demonstrate that an artificial solid-electrolyte interface layer consisting of an ultra-thin Al2O3 film, generated via atomic layer deposition (ALD) at the graphite surface, can successfully isolate the graphite from the electrolyte and inhibit the undesired reactions. Consequently, the capacity and cycling stability of the LNMO/graphite cell are drastically improved. After 300 cycles, the capacity retention of LNMO/graphite cell increases from 57.7% to 98.6% with the ALD-coated graphite. Furthermore, our findings provide valuable insights into the LNMO/graphite cell degradation and suggest a simple and robust, yet highly effective, approach for the practical viability of high-voltage lithium-ion batteries.},
doi = {10.1016/j.ensm.2021.09.033},
journal = {Energy Storage Materials},
number = ,
volume = 43,
place = {United States},
year = {Tue Sep 28 00:00:00 EDT 2021},
month = {Tue Sep 28 00:00:00 EDT 2021}
}
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Works referenced in this record:
A New Strategy to Stabilize Capacity and Insight into the Interface Behavior in Electrochemical Reaction of LiNi 0.5 Mn 1.5 O 4 /Graphite System for High-Voltage Lithium-Ion Batteries
journal, September 2017
- Wang, Hongqiang; Xie, Xuesong; Wei, Xiaolu
- ACS Applied Materials & Interfaces, Vol. 9, Issue 38
Fluorinated phosphazene derivative – A promising electrolyte additive for high voltage lithium ion batteries: From electrochemical performance to corrosion mechanism
journal, April 2018
- Liu, Jianwen; Song, Xin; Zhou, Lai
- Nano Energy, Vol. 46
Superconcentrated electrolytes for a high-voltage lithium-ion battery
journal, June 2016
- Wang, Jianhui; Yamada, Yuki; Sodeyama, Keitaro
- Nature Communications, Vol. 7, Issue 1
Facilitating the Operation of Lithium-Ion Cells with High-Nickel Layered Oxide Cathodes with a Small Dose of Aluminum
journal, April 2018
- Li, Jianyu; Li, Wangda; Wang, Shanyu
- Chemistry of Materials, Vol. 30, Issue 9
Crystal Chemistry and Electrochemistry of Li x Mn 1.5 Ni 0.5 O 4 Solid Solution Cathode Materials
journal, August 2017
- Kan, Wang Hay; Kuppan, Saravanan; Cheng, Lei
- Chemistry of Materials, Vol. 29, Issue 16
A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries
journal, October 2019
- Li, Jianyu; Manthiram, Arumugam
- Advanced Energy Materials, Vol. 9, Issue 45
Surface Reconstruction in Li-Rich Layered Oxides of Li-Ion Batteries
journal, September 2017
- Jarvis, Karalee; Wang, Chih-Chieh; Varela, Maria
- Chemistry of Materials, Vol. 29, Issue 18
Lithium bisoxalatodifluorophosphate (LiBODFP) as a multifunctional electrolyte additive for 5 V LiNi 0.5 Mn 1.5 O 4 -based lithium-ion batteries with enhanced electrochemical performance
journal, January 2019
- Yang, Tianxiang; Zeng, Huanna; Wang, Wenlian
- Journal of Materials Chemistry A, Vol. 7, Issue 14
Atomic-Scale Structure-Property Relationships in Lithium Ion Battery Electrode Materials
journal, July 2017
- Yang, Zhenzhong; Gu, Lin; Hu, Yong-Sheng
- Annual Review of Materials Research, Vol. 47, Issue 1
Overcoming the Challenges of 5 V Spinel LiNi 0.5 Mn 1.5 O 4 Cathodes with Solid Polymer Electrolytes
journal, October 2019
- Xu, Hantao; Zhang, Huanrui; Ma, Jun
- ACS Energy Letters, Vol. 4, Issue 12
A Long Cycle‐Life High‐Voltage Spinel Lithium‐Ion Battery Electrode Achieved by Site‐Selective Doping
journal, April 2020
- Liang, Gemeng; Wu, Zhibin; Didier, Christophe
- Angewandte Chemie International Edition, Vol. 59, Issue 26
High-nickel layered oxide cathodes for lithium-based automotive batteries
journal, January 2020
- Li, Wangda; Erickson, Evan M.; Manthiram, Arumugam
- Nature Energy, Vol. 5, Issue 1
Atomic layer deposition (ALD) of lithium fluoride (LiF) protective film on Li-ion battery LiMn1.5Ni0.5O4 cathode powder material
journal, February 2020
- Tiurin, Ortal; Solomatin, Nickolay; Auinat, Mahmud
- Journal of Power Sources, Vol. 448
Impact of the cycling temperature on electrode/electrolyte interfaces within Li4Ti5O12 vs LiMn2O4 cells
journal, February 2020
- Gauthier, Nicolas; Courrèges, Cécile; Demeaux, Julien
- Journal of Power Sources, Vol. 448
Hybrid Aqueous/Non-aqueous Electrolyte for Safe and High-Energy Li-Ion Batteries
journal, May 2018
- Wang, Fei; Borodin, Oleg; Ding, Michael S.
- Joule, Vol. 2, Issue 5
Influence of doping on the cation ordering and charge–discharge behavior of LiMn1.5Ni0.5−xMxO4 (M = Cr, Fe, Co, and Ga) spinels between 5.0 and 2.0 V
journal, January 2013
- Lee, Eun-Sung; Manthiram, Arumugam
- Journal of Materials Chemistry A, Vol. 1, Issue 9
Stabilized High-Voltage Cathodes via an F-Rich and Si-Containing Electrolyte Additive
journal, May 2020
- Li, Yuanqin; Wang, Kang; Chen, Jiawei
- ACS Applied Materials & Interfaces, Vol. 12, Issue 25
Dissolution, migration, and deposition of transition metal ions in Li-ion batteries exemplified by Mn-based cathodes – a critical review
journal, January 2018
- Zhan, Chun; Wu, Tianpin; Lu, Jun
- Energy & Environmental Science, Vol. 11, Issue 2
A Bifunctional Electrolyte Additive for High-Voltage LiNi 0.5 Mn 1.5 O 4 Positive Electrodes
journal, March 2019
- Lee, Tae Jin; Soon, Jiyong; Chae, Seulki
- ACS Applied Materials & Interfaces, Vol. 11, Issue 12
How Do Li Atoms Pass through the Al 2 O 3 Coating Layer during Lithiation in Li-ion Batteries?
journal, July 2013
- Jung, Sung Chul; Han, Young-Kyu
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 16
Understanding the capacity fading mechanism in LiNi0.5Mn1.5O4/graphite Li-ion batteries
journal, February 2013
- Kim, Jung-Hyun; Pieczonka, Nicholas P. W.; Li, Zicheng
- Electrochimica Acta, Vol. 90
Truncated octahedral LiNi0.5Mn1.5O4 cathode material for ultralong-life lithium-ion battery: Positive (100) surfaces in high-voltage spinel system
journal, December 2015
- Liu, Haidong; Kloepsch, Richard; Wang, Jun
- Journal of Power Sources, Vol. 300
A well-designed water-soluble binder enlightening the 5 V-class LiNi 0.5 Mn 1.5 O 4 cathodes
journal, January 2019
- Dong, Tiantian; Zhang, Huanrui; Ma, Yue
- Journal of Materials Chemistry A, Vol. 7, Issue 42
Decomposition of LiPF 6 in High Energy Lithium-Ion Batteries Studied with Online Electrochemical Mass Spectrometry
journal, January 2016
- Guéguen, Aurélie; Streich, Daniel; He, Minglong
- Journal of The Electrochemical Society, Vol. 163, Issue 6
Performance improvement and failure mechanism of LiNi 0.5 Mn 1.5 O 4 /graphite cells with biphenyl additive
journal, January 2014
- Xulai, Yang; Junlong, Xing; Xu, Liu
- Phys. Chem. Chem. Phys., Vol. 16, Issue 44
Cation Ordering and Oxygen Release in LiNi 0.5– x Mn 1.5+ x O 4– y (LNMO): In Situ Neutron Diffraction and Performance in Li Ion Full Cells
journal, April 2019
- Aktekin, Burak; Valvo, Mario; Smith, Ronald I.
- ACS Applied Energy Materials, Vol. 2, Issue 5
Evidence of loss of active lithium in titanium-doped LiNi0.5Mn1.5O4/graphite cells
journal, January 2015
- Höweling, Andres; Glatthaar, Sven; Nötzel, Dorit
- Journal of Power Sources, Vol. 274
Simulation of the surface structure of lithium manganese oxide spinel
journal, May 2011
- Benedek, R.; Thackeray, M. M.
- Physical Review B, Vol. 83, Issue 19
A reflection on lithium-ion battery cathode chemistry
journal, March 2020
- Manthiram, Arumugam
- Nature Communications, Vol. 11, Issue 1
Unravelling the Role of Electrochemically Active FePO 4 Coating by Atomic Layer Deposition for Increased High-Voltage Stability of LiNi 0.5 Mn 1.5 O 4 Cathode Material
journal, March 2015
- Xiao, Biwei; Liu, Jian; Sun, Qian
- Advanced Science, Vol. 2, Issue 5
Lithium Polyacrylate (LiPAA) as an Advanced Binder and a Passivating Agent for High-Voltage Li-Ion Batteries
journal, September 2015
- Pieczonka, Nicholas P. W.; Borgel, Valentina; Ziv, Baruch
- Advanced Energy Materials, Vol. 5, Issue 23
Enabling high areal capacity for Co-free high voltage spinel materials in next-generation Li-ion batteries
journal, October 2020
- Li, Weikang; Cho, Yoon-Gyo; Yao, Weiliang
- Journal of Power Sources, Vol. 473
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
A carbonate-free, sulfone-based electrolyte for high-voltage Li-ion batteries
journal, May 2018
- Alvarado, Judith; Schroeder, Marshall A.; Zhang, Minghao
- Materials Today, Vol. 21, Issue 4
Manipulation of an ionic and electronic conductive interface for highly-stable high-voltage cathodes
journal, November 2019
- Deng, Sixu; Wang, Biqiong; Yuan, Yifei
- Nano Energy, Vol. 65
Toward Long-Life, Ultrahigh-Nickel Layered Oxide Cathodes for Lithium-Ion Batteries: Optimizing the Interphase Chemistry with a Dual-Functional Polymer
journal, December 2019
- Li, Jianyu; Chang, Chi-Hao; Manthiram, Arumugam
- Chemistry of Materials, Vol. 32, Issue 2
Room‐Temperature All‐Liquid‐Metal Batteries Based on Fusible Alloys with Regulated Interfacial Chemistry and Wetting
journal, June 2020
- Ding, Yu; Guo, Xuelin; Qian, Yumin
- Advanced Materials, Vol. 32, Issue 30
SEI layer-forming additives for LiNi0.5Mn1.5O4/graphite 5V Li-ion batteries
journal, April 2007
- Lee, Hochun; Choi, Seungdon; Choi, Sanghoon
- Electrochemistry Communications, Vol. 9, Issue 4
Garnet Electrolyte with an Ultralow Interfacial Resistance for Li-Metal Batteries
journal, April 2018
- Li, Yutao; Chen, Xi; Dolocan, Andrei
- Journal of the American Chemical Society, Vol. 140, Issue 20
Crystallographic facet- and size-controllable synthesis of spinel LiNi 0.5 Mn 1.5 O 4 with excellent cyclic stability as cathode of high voltage lithium ion battery
journal, January 2014
- Lin, H. B.; Zhang, Y. M.; Rong, H. B.
- Journal of Materials Chemistry A, Vol. 2, Issue 30
Nanoscale Manipulation of Spinel Lithium Nickel Manganese Oxide Surface by Multisite Ti Occupation as High-Performance Cathode
journal, October 2017
- Xiao, Biwei; Liu, Hanshuo; Liu, Jian
- Advanced Materials, Vol. 29, Issue 47
Challenges and Approaches for High-Voltage Spinel Lithium-Ion Batteries
journal, May 2014
- Kim, Jung-Hyun; Pieczonka, Nicholas P. W.; Yang, Li
- ChemPhysChem, Vol. 15, Issue 10
Layered lithium cobalt oxide cathodes
journal, March 2021
- Manthiram, Arumugam; Goodenough, John B.
- Nature Energy, Vol. 6, Issue 3
Nano‐Sized AlPO 4 Coating Layer on Graphite Powder to Improve the Electrochemical Properties of High‐Voltage Graphite/LiNi 0.5 Mn 1.5 O 4 Li‐Ion Cells
journal, June 2019
- Zeng, Huanna; He, Jia; Fang, Danyang
- Energy Technology, Vol. 7, Issue 9
Understanding Transition-Metal Dissolution Behavior in LiNi 0.5 Mn 1.5 O 4 High-Voltage Spinel for Lithium Ion Batteries
journal, July 2013
- Pieczonka, Nicholas P. W.; Liu, Zhongyi; Lu, Peng
- The Journal of Physical Chemistry C, Vol. 117, Issue 31
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
Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries
journal, January 2018
- Suo, Liumin; Xue, Weijiang; Gobet, Mallory
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 6
Review—Multifunctional Separators: A Promising Approach for Improving the Durability and Performance of Li-Ion Batteries
journal, January 2019
- Banerjee, Anjan; Ziv, Baruch; Shilina, Yuliya
- Journal of The Electrochemical Society, Vol. 166, Issue 3
Factors Influencing the Electrochemical Properties of High-Voltage Spinel Cathodes: Relative Impact of Morphology and Cation Ordering
journal, July 2013
- Chemelewski, Katharine R.; Lee, Eun-Sung; Li, Wei
- Chemistry of Materials, Vol. 25, Issue 14
Crystal engineering of TMPOx-coated LiNi0.5Mn1.5O4 cathodes for high-performance lithium-ion batteries
journal, October 2020
- Kuenzel, Matthias; Kim, Guk-Tae; Zarrabeitia, Maider
- Materials Today, Vol. 39