Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material
Abstract
With the proliferation of market demand for lithium-ion batteries (LIBs) over the past decades, battery recycling has aroused extensive attention due to the environmental, supply, and economic issues caused by waste batteries. Here, the hydrometallurgical recycling method has been widely adopted to recover cathode materials as a result of its wide applicability and high productivity. However, it is hard to completely eliminate impurities such as copper, aluminum, and carbon, which could bring significant impacts on recovered materials. Here, the influence of the carbon impurity on recovered LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode material is systematically investigated. It shows that the carbon impurity promotes nucleation during coprecipitation and forms holes in the cathode secondary particles after sintering which could enhance cyclability of the NCM622 cathode. The cathode with 0.2 atom % of carbon impurity displays the highest capacity of 159.9 mAh/g with a striking capacity retention rate of 97.9% after 100 cycles at 0.33C, but performs worse at high rates. Nonetheless, excess carbon (5 atom %) results in severe cation disorder and lattice distortion which significantly deteriorates the electrochemical properties of the NCM622 cathode. Therefore, it is important to strictly control carbon impurity during the recycling process for spent LIBs.
- Authors:
-
[1];
[1];
[1]
- Worcester Polytechnic Inst., MA (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
- OSTI Identifier:
- 1781800
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Sustainable Chemistry & Engineering
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 17; Journal ID: ISSN 2168-0485
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Carbon impurity; Electrochemistry; Hydrometallurgical recycling; LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode; Lithium-ion batteries; Impurities; Precursors; Nanoparticles; Electrodes; Transition metals
Citation Formats
Zheng, Yadong, Zhang, Ruihan, Vanaphuti, Panawan, Fu, Jinzhao, Yang, Zhenzhen, and Wang, Yan. Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material. United States: N. p., 2021.
Web. doi:10.1021/acssuschemeng.1c01510.
Zheng, Yadong, Zhang, Ruihan, Vanaphuti, Panawan, Fu, Jinzhao, Yang, Zhenzhen, & Wang, Yan. Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material. United States. https://doi.org/10.1021/acssuschemeng.1c01510
Zheng, Yadong, Zhang, Ruihan, Vanaphuti, Panawan, Fu, Jinzhao, Yang, Zhenzhen, and Wang, Yan. Thu .
"Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material". United States. https://doi.org/10.1021/acssuschemeng.1c01510. https://www.osti.gov/servlets/purl/1781800.
@article{osti_1781800,
title = {Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material},
author = {Zheng, Yadong and Zhang, Ruihan and Vanaphuti, Panawan and Fu, Jinzhao and Yang, Zhenzhen and Wang, Yan},
abstractNote = {With the proliferation of market demand for lithium-ion batteries (LIBs) over the past decades, battery recycling has aroused extensive attention due to the environmental, supply, and economic issues caused by waste batteries. Here, the hydrometallurgical recycling method has been widely adopted to recover cathode materials as a result of its wide applicability and high productivity. However, it is hard to completely eliminate impurities such as copper, aluminum, and carbon, which could bring significant impacts on recovered materials. Here, the influence of the carbon impurity on recovered LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode material is systematically investigated. It shows that the carbon impurity promotes nucleation during coprecipitation and forms holes in the cathode secondary particles after sintering which could enhance cyclability of the NCM622 cathode. The cathode with 0.2 atom % of carbon impurity displays the highest capacity of 159.9 mAh/g with a striking capacity retention rate of 97.9% after 100 cycles at 0.33C, but performs worse at high rates. Nonetheless, excess carbon (5 atom %) results in severe cation disorder and lattice distortion which significantly deteriorates the electrochemical properties of the NCM622 cathode. Therefore, it is important to strictly control carbon impurity during the recycling process for spent LIBs.},
doi = {10.1021/acssuschemeng.1c01510},
journal = {ACS Sustainable Chemistry & Engineering},
number = 17,
volume = 9,
place = {United States},
year = {Thu Apr 22 00:00:00 EDT 2021},
month = {Thu Apr 22 00:00:00 EDT 2021}
}
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Works referenced in this record:
Performance of layered Li(Ni1/3Co1/3Mn1/3)O2 as cathode for Li-ion batteries
journal, November 2002
- Shaju, K. M.; Subba Rao, G. V.; Chowdari, B. V. R.
- Electrochimica Acta, Vol. 48, Issue 2
Issues and challenges facing rechargeable lithium batteries
journal, November 2001
- Tarascon, J.-M.; Armand, M.
- Nature, Vol. 414, Issue 6861, p. 359-367
Metal Oxide Hollow Nanostructures for Lithium-ion Batteries
journal, March 2012
- Wang, Zhiyu; Zhou, Liang; David Lou, Xiong Wen
- Advanced Materials, Vol. 24, Issue 14, p. 1903-1911
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
A New Coating Method for Alleviating Surface Degradation of LiNi 0.6 Co 0.2 Mn 0.2 O 2 Cathode Material: Nanoscale Surface Treatment of Primary Particles
journal, February 2015
- Kim, Hyejung; Kim, Min Gyu; Jeong, Hu Young
- Nano Letters, Vol. 15, Issue 3
LiNi0.5Co0.2Mn0.3O2 hollow microspheres-synthesis, characterization and application as cathode materials for power lithium ion batteries
journal, February 2018
- Zhao, Xinxin; An, Liwei; Sun, Jiachen
- Journal of Electroanalytical Chemistry, Vol. 810
AC Impedance Analysis of Polycrystalline Insertion Electrodes: Application to Li[sub 1−x]CoO[sub 2]
journal, January 1985
- Thomas, M. G. S. R.
- Journal of The Electrochemical Society, Vol. 132, Issue 7
Synthesis and characterization of LiNi0.6Mn0.4−xCoxO2 as cathode materials for Li-ion batteries
journal, April 2009
- Li, Jiangang; Wang, Li; Zhang, Qian
- Journal of Power Sources, Vol. 189, Issue 1
LiNi1/3Co1/3Mn1/3O2 hollow nano-micro hierarchical microspheres with enhanced performances as cathodes for lithium-ion batteries
journal, January 2013
- Li, Jili; Cao, Chuanbao; Xu, Xingyan
- Journal of Materials Chemistry A, Vol. 1, Issue 38
The effect of Fe as an impurity element for sustainable resynthesis of Li[Ni1/3Co1/3Mn1/3]O2 cathode material from spent lithium-ion batteries
journal, February 2019
- Park, Sanghyuk; Kim, Duho; Ku, Heesuk
- Electrochimica Acta, Vol. 296
NiO nanorings and their unexpected catalytic property for CO oxidation
journal, January 2006
- Wang, Dingsheng; Xu, Run; Wang, Xun
- Nanotechnology, Vol. 17, Issue 4
Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries
journal, January 2014
- Lee, J.; Urban, A.; Li, X.
- Science, Vol. 343, Issue 6170
R factors in Rietveld analysis: How good is good enough?
journal, March 2006
- Toby, Brian H.
- Powder Diffraction, Vol. 21, Issue 1
Cathodes of spent Li-ion batteries: Dissolution with phosphoric acid and recovery of lithium and cobalt from leach liquors
journal, January 2017
- Pinna, Eliana G.; Ruiz, M. C.; Ojeda, Manuel W.
- Hydrometallurgy, Vol. 167
Electronic Structure and Comparative Properties of LiNi x Mn y Co z O 2 Cathode Materials
journal, March 2017
- Sun, Hong; Zhao, Kejie
- The Journal of Physical Chemistry C, Vol. 121, Issue 11
Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries
journal, April 2019
- de Biasi, Lea; Schwarz, Björn; Brezesinski, Torsten
- Advanced Materials, Vol. 31, Issue 26
Systematic Study of Different Anion Doping on the Electrochemical Performance of Cobalt-Free Lithium–Manganese-Rich Layered Cathode
journal, April 2020
- Vanaphuti, Panawan; Bong, Sungyool; Ma, Lu
- ACS Applied Energy Materials, Vol. 3, Issue 5
Mitigating storage-induced degradation of Ni-rich LiNi0.8Co0.1Mn0.1O2 cathode material by surface tuning with phosphate
journal, August 2019
- Ryu, Won-Gyue; Shin, Hyun-Seop; Park, Min-Sik
- Ceramics International, Vol. 45, Issue 11
Different strategies of introduction of lithium ions into nickel‑manganese‑cobalt carbonate resulting in LiNi0.6Mn0.2Co0.2O2 (NMC622) cathode material for Li-ion batteries
journal, May 2020
- Zybert, Magdalena; Ronduda, Hubert; Szczęsna, Anna
- Solid State Ionics, Vol. 348
Improved electrochemical and thermal properties of nickel rich LiNi0.6Co0.2Mn0.2O2 cathode materials by SiO2 coating
journal, May 2015
- Cho, Woosuk; Kim, Sang-Min; Song, Jun Ho
- Journal of Power Sources, Vol. 282
Li-ion battery materials: present and future
journal, June 2015
- Nitta, Naoki; Wu, Feixiang; Lee, Jung Tae
- Materials Today, Vol. 18, Issue 5
Quantitative analysis of Ni2+/Ni3+ in Li[NixMnyCoz]O2 cathode materials: Non-linear least-squares fitting of XPS spectra
journal, May 2018
- Fu, Zewei; Hu, Juntao; Hu, Wenlong
- Applied Surface Science, Vol. 441
A brief review on hydrometallurgical technologies for recycling spent lithium-ion batteries: Technologies for recycling spent lithium-ion batteries
journal, April 2013
- Chagnes, Alexandre; Pospiech, Beata
- Journal of Chemical Technology & Biotechnology, Vol. 88, Issue 7
Silicon carbide nano-fibers in-situ grown on carbon fibers for enhanced microwave absorption properties
journal, May 2017
- Zhou, Wei; Long, Lan; Xiao, Peng
- Ceramics International, Vol. 43, Issue 7
Li ion kinetic studies on spinel cathodes, Li(M1/6Mn11/6)O4 (M = Mn, Co, CoAl) by GITT and EIS
journal, November 2002
- Shaju, K. M.; Subba Rao, G. V.; Chowdari, B. V. R.
- Journal of Materials Chemistry, Vol. 13, Issue 1
Effect of impurities caused by a recycling process on the electrochemical performance of Li[Ni0.33Co0.33Mn0.33]O2
journal, July 2014
- Krüger, S.; Hanisch, C.; Kwade, A.
- Journal of Electroanalytical Chemistry, Vol. 726
Surface phenomena of high energy Li(Ni1/3Co1/3Mn1/3)O2/graphite cells at high temperature and high cutoff voltages
journal, December 2014
- Liu, Ting; Garsuch, Arnd; Chesneau, Frederick
- Journal of Power Sources, Vol. 269
A novel method to recycle mixed cathode materials for lithium ion batteries
journal, January 2013
- Zou, Haiyang; Gratz, Eric; Apelian, Diran
- Green Chemistry, Vol. 15, Issue 5
Comparison of structure and electrochemistry of Al- and Fe-doped LiNi1/3Co1/3Mn1/3O2
journal, May 2006
- Liu, Daotan; Wang, Zhaoxiang; Chen, Liquan
- Electrochimica Acta, Vol. 51, Issue 20
A combined recovery process of metals in spent lithium-ion batteries
journal, November 2009
- Li, Jinhui; Shi, Pixing; Wang, Zefeng
- Chemosphere, Vol. 77, Issue 8
Synthesis and electrochemical properties of LiNi0.8CoxMn0.2-xO2 positive-electrode material for lithium-ion batteries
journal, September 2016
- Zhong, Shengwen; Lai, Meizhen; Yao, Wenli
- Electrochimica Acta, Vol. 212
Unravelling the growth mechanism of hierarchically structured Ni1/3Co1/3Mn1/3(OH)2 and their application as precursors for high-power cathode materials
journal, April 2017
- Hua, Weibo; Liu, Wenyuan; Chen, Mingzhe
- Electrochimica Acta, Vol. 232
Electron Transfer Mechanisms upon Lithium Deintercalation from LiCoO 2 to CoO 2 Investigated by XPS
journal, January 2008
- Dahéron, L.; Dedryvère, R.; Martinez, H.
- Chemistry of Materials, Vol. 20, Issue 2
Effect of precursor and synthesis temperature on the structural and electrochemical properties of Li(Ni0.5Co0.2Mn0.3)O2
journal, July 2012
- Wu, Kuichen; Wang, Fei; Gao, Lulu
- Electrochimica Acta, Vol. 75
Systematic Study of Al Impurity for NCM622 Cathode Materials
journal, June 2020
- Zhang, Ruihan; Zheng, Yadong; Yao, Zeyi
- ACS Sustainable Chemistry & Engineering, Vol. 8, Issue 26
Structural evolution and capacity degradation mechanism of LiNi0.6Mn0.2Co0.2O2 cathode materials
journal, October 2018
- Ruan, Yanli; Song, Xiangyun; Fu, Yanbao
- Journal of Power Sources, Vol. 400
Copper Impurity Effects on LiNi 1/3 Mn 1/3 Co 1/3 O 2 Cathode Material
journal, September 2015
- Sa, Qina; Heelan, Joseph A.; Lu, Yuan
- ACS Applied Materials & Interfaces, Vol. 7, Issue 37
Double-shelled hollow microspheres of LiMn2O4 for high-performance lithium ion batteries
journal, January 2011
- Ding, Yuan-Li; Zhao, Xin-Bing; Xie, Jian
- Journal of Materials Chemistry, Vol. 21, Issue 26
Analysis of the Growth Mechanism of Coprecipitated Spherical and Dense Nickel, Manganese, and Cobalt-Containing Hydroxides in the Presence of Aqueous Ammonia
journal, April 2009
- van Bommel, Andrew; Dahn, J. R.
- Chemistry of Materials, Vol. 21, Issue 8
High Performance Cathode Recovery from Different Electric Vehicle Recycling Streams
journal, September 2018
- Zheng, Zhangfeng; Chen, Mengyuan; Wang, Qiang
- ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 11
Influence of calcination atmosphere on structure and electrochemical behavior of LiNi0.6Co0.2Mn0.2O2 cathode material for lithium-ion batteries
journal, March 2017
- Yuan, Jing; Wen, Jianwu; Zhang, Jinbo
- Electrochimica Acta, Vol. 230
A reflection on lithium-ion battery cathode chemistry
journal, March 2020
- Manthiram, Arumugam
- Nature Communications, Vol. 11, Issue 1
Enabling sustainable critical materials for battery storage through efficient recycling and improved design: A perspective
journal, July 2020
- Tan, Darren H. S.; Xu, Panpan; Chen, Zheng
- MRS Energy & Sustainability, Vol. 7, Issue 1
Development of a recycling process for Li-ion batteries
journal, June 2012
- Georgi-Maschler, T.; Friedrich, B.; Weyhe, R.
- Journal of Power Sources, Vol. 207
Understanding fundamental effects of Cu impurity in different forms for recovered LiNi0.6Co0.2Mn0.2O2 cathode materials
journal, December 2020
- Zhang, Ruihan; Meng, Zifei; Ma, Xiaotu
- Nano Energy, Vol. 78
Co–precipitation synthesis of Ni0.6Co0.2Mn0.2(OH)2 precursor and characterization of LiNi0.6Co0.2Mn0.2O2 cathode material for secondary lithium batteries
journal, June 2014
- Liang, Longwei; Du, Ke; Peng, Zhongdong
- Electrochimica Acta, Vol. 130
Solvothermal synthesis of surfactant free spherical nickel hydroxide/graphene oxide composite for supercapacitor application
journal, October 2017
- Khaleed, A. A.; Bello, A.; Dangbegnon, J. K.
- Journal of Alloys and Compounds, Vol. 721
Effect of iron doping on LiNi0.35Co0.30Mn0.35O2
journal, November 2018
- Mi, Chen; Han, Enshan; Li, Ling
- Solid State Ionics, Vol. 325
Positive Electrode Materials for Li-Ion and Li-Batteries †
journal, February 2010
- Ellis, Brian L.; Lee, Kyu Tae; Nazar, Linda F.
- Chemistry of Materials, Vol. 22, Issue 3
Unraveling Na and F coupling effects in stabilizing Li, Mn-rich layered oxide cathodes via local ordering modification
journal, October 2020
- Vanaphuti, Panawan; Bai, Jianming; Ma, Lu
- Energy Storage Materials, Vol. 31
A closed loop process for recycling spent lithium ion batteries
journal, September 2014
- Gratz, Eric; Sa, Qina; Apelian, Diran
- Journal of Power Sources, Vol. 262, p. 255-262
Synthesis of high performance LiNi1/3Mn1/3Co1/3O2 from lithium ion battery recovery stream
journal, May 2015
- Sa, Qina; Gratz, Eric; He, Meinan
- Journal of Power Sources, Vol. 282
Synthesis of Diverse LiNixMnyCozO2 Cathode Materials from Lithium Ion Battery Recovery Stream
journal, April 2016
- Sa, Qina; Gratz, Eric; Heelan, Joseph A.
- Journal of Sustainable Metallurgy, Vol. 2, Issue 3
Synthetic optimization of Li[Ni1/3Co1/3Mn1/3]O2 via co-precipitation
journal, December 2004
- Lee, M. -H.; Kang, Y. -J.; Myung, S. -T.
- Electrochimica Acta, Vol. 50, Issue 4
Retarded phase transition by fluorine doping in Li-rich layered Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 cathode material
journal, June 2015
- Li, L.; Song, B. H.; Chang, Y. L.
- Journal of Power Sources, Vol. 283
Effect of Cu substitution on structures and electrochemical properties of Li[NiCo 1−x Cu x Mn] 1/3 O 2 as cathode materials for lithium ion batteries
journal, January 2015
- Wu, Zhao-Jin; Wang, Dong; Gao, Zhi-Fang
- Dalton Transactions, Vol. 44, Issue 42
1D Nb-doped LiNi1/3Co1/3Mn1/3O2 nanostructures as excellent cathodes for Li-ion battery
journal, February 2019
- Lv, Congjie; Yang, Jing; Peng, Yi
- Electrochimica Acta, Vol. 297
Recycling End-of-Life Electric Vehicle Lithium-Ion Batteries
journal, November 2019
- Chen, Mengyuan; Ma, Xiaotu; Chen, Bin
- Joule, Vol. 3, Issue 11
Promise and reality of post-lithium-ion batteries with high energy densities
journal, March 2016
- Choi, Jang Wook; Aurbach, Doron
- Nature Reviews Materials, Vol. 1, Issue 4
Study on the reversible capacity loss of layered oxide cathode during low-temperature operation
journal, February 2017
- Li, Yiyang; Qian, Kun; He, Yan-Bing
- Journal of Power Sources, Vol. 342
Closed Loop Recycling of Electric Vehicle Batteries to Enable Ultra-high Quality Cathode Powder
journal, February 2019
- Chen, Mengyuan; Zheng, Zhangfeng; Wang, Qiang
- Scientific Reports, Vol. 9, Issue 1
Hierarchical Porous LiNi1/3Co1/3Mn1/3O2 Nano-/Micro Spherical Cathode Material: Minimized Cation Mixing and Improved Li+ Mobility for Enhanced Electrochemical Performance
journal, May 2016
- Chen, Zhen; Wang, Jin; Chao, Dongliang
- Scientific Reports, Vol. 6, Issue 1