Valence Effects of Fe Impurity for Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Materials
Abstract
Iron impurities are generally included in the obtained leaching liquor solution during the hydrometallurgical recycling method of spent lithium-ion batteries (LIBs) due to the usage of iron in battery casings and machinery parts of recycling equipment, which would definitely affect the physical and electrochemical features of the recovered active materials. In this paper, the effects of iron impurity with different valence states (Fe2+ and Fe3+) and gradient concentrations (0.2, 1.0, and 5.0 at. %) for the obtained LiNi0.6Co0.2Mn0.2O2 (NCM622) cathodes are fully studied. It is found that Fe3+ impurity could easily lower the tap density and average size of NCM622 particles and even introduce some impurity phases in the NCM622 structure at high concentration (5.0 at. %), leading to much lower specific capacity, worse rate capability, and cycling performance of the Fe3+-based NCM622 cathode. On contrast, with certain concentrations of Fe2+ impurity (0.2 and 1.0 at. %), the NCM622 cathode material exhibits comparable and much better electrochemical properties compared with the virgin NCM622 materials. Based on these results, the valence of Fe impurity should be considered and controlled as well as its concentration during the recycling process design for spent LIBs.
- Authors:
-
[1];
[1];
[1];
[2];
[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:
- 1840965
- Alternate Identifier(s):
- OSTI ID: 1840909
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Energy Materials
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 9; Journal ID: ISSN 2574-0962
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; recovered LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode materials; iron impurities; spent LIB recycling process; cation mixing degree; XPS depth profiling technique; impurities; precursors; materials; electrodes; ions
Citation Formats
Zhang, Ruihan, Zheng, Yadong, Vanaphuti, Panawan, Liu, Yangtao, Fu, Jinzhao, Yao, Zeyi, Ma, Xiaotu, Chen, Mengyuan, Yang, Zhenzhen, Lin, Yulin, Wen, Jianguo, and Wang, Yan. Valence Effects of Fe Impurity for Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Materials. United States: N. p., 2021.
Web. doi:10.1021/acsaem.1c02281.
Zhang, Ruihan, Zheng, Yadong, Vanaphuti, Panawan, Liu, Yangtao, Fu, Jinzhao, Yao, Zeyi, Ma, Xiaotu, Chen, Mengyuan, Yang, Zhenzhen, Lin, Yulin, Wen, Jianguo, & Wang, Yan. Valence Effects of Fe Impurity for Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Materials. United States. https://doi.org/10.1021/acsaem.1c02281
Zhang, Ruihan, Zheng, Yadong, Vanaphuti, Panawan, Liu, Yangtao, Fu, Jinzhao, Yao, Zeyi, Ma, Xiaotu, Chen, Mengyuan, Yang, Zhenzhen, Lin, Yulin, Wen, Jianguo, and Wang, Yan. Thu .
"Valence Effects of Fe Impurity for Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Materials". United States. https://doi.org/10.1021/acsaem.1c02281. https://www.osti.gov/servlets/purl/1840965.
@article{osti_1840965,
title = {Valence Effects of Fe Impurity for Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Materials},
author = {Zhang, Ruihan and Zheng, Yadong and Vanaphuti, Panawan and Liu, Yangtao and Fu, Jinzhao and Yao, Zeyi and Ma, Xiaotu and Chen, Mengyuan and Yang, Zhenzhen and Lin, Yulin and Wen, Jianguo and Wang, Yan},
abstractNote = {Iron impurities are generally included in the obtained leaching liquor solution during the hydrometallurgical recycling method of spent lithium-ion batteries (LIBs) due to the usage of iron in battery casings and machinery parts of recycling equipment, which would definitely affect the physical and electrochemical features of the recovered active materials. In this paper, the effects of iron impurity with different valence states (Fe2+ and Fe3+) and gradient concentrations (0.2, 1.0, and 5.0 at. %) for the obtained LiNi0.6Co0.2Mn0.2O2 (NCM622) cathodes are fully studied. It is found that Fe3+ impurity could easily lower the tap density and average size of NCM622 particles and even introduce some impurity phases in the NCM622 structure at high concentration (5.0 at. %), leading to much lower specific capacity, worse rate capability, and cycling performance of the Fe3+-based NCM622 cathode. On contrast, with certain concentrations of Fe2+ impurity (0.2 and 1.0 at. %), the NCM622 cathode material exhibits comparable and much better electrochemical properties compared with the virgin NCM622 materials. Based on these results, the valence of Fe impurity should be considered and controlled as well as its concentration during the recycling process design for spent LIBs.},
doi = {10.1021/acsaem.1c02281},
journal = {ACS Applied Energy Materials},
number = 9,
volume = 4,
place = {United States},
year = {Thu Sep 16 00:00:00 EDT 2021},
month = {Thu Sep 16 00:00:00 EDT 2021}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
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:
A comparative study on electrochemical cycling stability of lithium rich layered cathode materials Li 1.2 Ni 0.13 M 0.13 Mn 0.54 O 2 where M = Fe or Co
journal, August 2016
- Laisa, C. P.; Nanda Kumar, A. K.; Selva Chandrasekaran, S.
- Journal of Power Sources, Vol. 324
Recycling of lithium-ion batteries: Recent advances and perspectives
journal, September 2018
- Huang, Bin; Pan, Zhefei; Su, Xiangyu
- Journal of Power Sources, Vol. 399
Green and facile synthesis of porous ZnCO3 as a novel anode material for advanced lithium-ion batteries
journal, March 2014
- Zhang, Ruihan; Zhang, Fan; Feng, Jinkui
- Materials Letters, Vol. 118
Pyrometallurgical recycling of Li-ion, Ni–Cd and Ni–MH batteries: A minireview
journal, August 2020
- Assefi, Mohammad; Maroufi, Samane; Yamauchi, Yusuke
- Current Opinion in Green and Sustainable Chemistry, Vol. 24
Structural Analysis of Li2MnO3 and Related Li-Mn-O Materials
journal, January 2011
- Yu, Denis Y. W.; Yanagida, Katsunori
- Journal of The Electrochemical Society, Vol. 158, Issue 9
Temperature Dependence of Oxygen Release from LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) Cathode Materials for Li-Ion Batteries
journal, January 2018
- Jung, Roland; Strobl, Philipp; Maglia, Filippo
- Journal of The Electrochemical Society, Vol. 165, Issue 11
Efficient Li-Metal Plating/Stripping in Carbonate Electrolytes Using a LiNO 3 -Gel Polymer Electrolyte, Monitored by Operando Neutron Depth Profiling
journal, May 2019
- Liu, Ming; Cheng, Zhu; Qian, Kun
- Chemistry of Materials, Vol. 31, Issue 12
Enhanced Electrochemical Performance of the Lithium-Manganese-Rich Cathode for Li-Ion Batteries with Na and F CoDoping
journal, September 2019
- Vanaphuti, Panawan; Chen, Jiajun; Cao, Jiayu
- ACS Applied Materials & Interfaces, Vol. 11, Issue 41
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
The Ultrafast Laser Ablation of Li(Ni0.6Mn0.2Co0.2)O2 Electrodes with High Mass Loading
journal, September 2019
- Zhu, Penghui; Seifert, Hans Jürgen; Pfleging, Wilhelm
- Applied Sciences, Vol. 9, Issue 19
Mathematical modeling and numerical analysis of alkaline zinc-iron flow batteries for energy storage applications
journal, February 2021
- Chen, Ziqi; Yu, Wentao; Liu, Yongfu
- Chemical Engineering Journal, Vol. 405
Environmental feasibility of secondary use of electric vehicle lithium-ion batteries in communication base stations
journal, May 2020
- Yang, Jie; Gu, Fu; Guo, Jianfeng
- Resources, Conservation and Recycling, Vol. 156
Incorporation of Cu into Li[Ni1/3Co1/3Mn1/3]O2 cathode: Elucidating its electrochemical properties and stability
journal, October 2018
- Jo, Minsang; Park, Sanghyuk; Song, Junho
- Journal of Alloys and Compounds, Vol. 764
Influence of Fe(III) doping on the crystal structure and properties of hydrothermally prepared β-Ni(OH)2 nanostructures
journal, June 2018
- Krehula, S.; Ristić, M.; Wu, C.
- Journal of Alloys and Compounds, Vol. 750
High-resolution X-ray diffraction, DIFFaX, NMR and first principles study of disorder in the Li2MnO3–Li[Ni1/2Mn1/2]O2 solid solution
journal, September 2005
- Bréger, Julien; Jiang, Meng; Dupré, Nicolas
- Journal of Solid State Chemistry, Vol. 178, Issue 9, p. 2575-2585
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
Porous lithium rich Li 1.2 Mn 0.54 Ni 0.22 Fe 0.04 O 2 prepared by microemulsion route as a high capacity and high rate capability positive electrode material
journal, October 2014
- Penki, Tirupathi Rao; Shanmughasundaram, D.; Munichandraiah, N.
- Electrochimica Acta, Vol. 143
Controlling the Lithium-Metal Growth To Enable Low-Lithium-Metal-Excess All-Solid-State Lithium-Metal Batteries
journal, May 2020
- Liu, Ming; Wang, Chao; Cheng, Zhu
- ACS Materials Letters, Vol. 2, Issue 7
Structurally stabilized LiNi0.5Mn1.5O4 with enhanced electrochemical properties through nitric acid treatment
journal, May 2013
- Park, Jun Soo; Roh, Kwang Chul; Lee, Jae-Won
- Journal of Power Sources, Vol. 230
New interpretations of XPS spectra of nickel metal and oxides
journal, May 2006
- Grosvenor, Andrew P.; Biesinger, Mark C.; Smart, Roger St. C.
- Surface Science, Vol. 600, Issue 9
A review on the key issues for lithium-ion battery management in electric vehicles
journal, March 2013
- Lu, Languang; Han, Xuebing; Li, Jianqiu
- Journal of Power Sources, Vol. 226, p. 272-288
Superior cycling life of Li–S batteries with high sulfur loading enabled by a bifunctional layered-MoO3 cathode
journal, October 2019
- Zhang, Ruihan; Wu, Maochun; Fan, Xinzhuang
- Journal of Power Sources, Vol. 436
Sustainable Recycling Technology for Li-Ion Batteries and Beyond: Challenges and Future Prospects
journal, January 2020
- Fan, Ersha; Li, Li; Wang, Zhenpo
- Chemical Reviews, Vol. 120, Issue 14
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
Li/Fe substitution in Li-rich Ni, Co, Mn oxides for enhanced electrochemical performance as cathode materials
journal, January 2019
- Billaud, Juliette; Sheptyakov, Denis; Sallard, Sébastien
- Journal of Materials Chemistry A, Vol. 7, Issue 25
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
Recycling Strategies for Spent Li-Ion Battery Mixed Cathodes
journal, August 2018
- Natarajan, Subramanian; Aravindan, Vanchiappan
- ACS Energy Letters, Vol. 3, Issue 9
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
Degradation of electric vehicle lithium-ion batteries in electricity grid services
journal, December 2020
- Elliott, Mark; Swan, Lukas G.; Dubarry, Matthieu
- Journal of Energy Storage, Vol. 32
Recycling metals from lithium ion battery by mechanical separation and vacuum metallurgy
journal, September 2017
- Xiao, Jiefeng; Li, Jia; Xu, Zhengming
- Journal of Hazardous Materials, Vol. 338
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
The synthesis, characterization and electrochemical behavior of the layered LiNi0.4Mn0.4Co0.2O2 compound
journal, January 2004
- Ngala, J. Katana; Chernova, Natasha A.; Ma, Miaomiao
- Journal of Materials Chemistry, Vol. 14, Issue 2
Recycling Chain for Spent Lithium-Ion Batteries
journal, February 2020
- Werner, Denis; Peuker, Urs Alexander; Mütze, Thomas
- Metals, Vol. 10, Issue 3
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
Enhanced cyclability and safety performance of LiNi0.6Co0.2Mn0.2O2 at elevated temperature by AlPO4 modification
journal, November 2019
- Tang, Wenjie; Peng, Zhenfeng; Shi, Yanli
- Journal of Alloys and Compounds, Vol. 810
Examining different recycling processes for lithium-ion batteries
journal, February 2019
- Ciez, Rebecca E.; Whitacre, J. F.
- Nature Sustainability, Vol. 2, Issue 2
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
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
Current and Prospective Li-Ion Battery Recycling and Recovery Processes
journal, June 2016
- Heelan, Joseph; Gratz, Eric; Zheng, Zhangfeng
- JOM, Vol. 68, Issue 10
Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials
journal, February 2008
- Yamashita, Toru; Hayes, Peter
- Applied Surface Science, Vol. 254, Issue 8
Nickel hydroxides and related materials: a review of their structures, synthesis and properties
journal, February 2015
- Hall, David S.; Lockwood, David J.; Bock, Christina
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 471, Issue 2174
Tandem Interface and Bulk Li-Ion Transport in a Hybrid Solid Electrolyte with Microsized Active Filler
journal, August 2019
- Liu, Ming; Cheng, Zhu; Ganapathy, Swapna
- ACS Energy Letters, Vol. 4, Issue 9
Techno-economic and environmental disassembly planning of lithium-ion electric vehicle battery packs for remanufacturing
journal, March 2020
- Alfaro-Algaba, M.; Ramirez, F. Javier
- Resources, Conservation and Recycling, Vol. 154
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
Facile Fabrication of Ethoxy-Functional Polysiloxane Wrapped LiNi 0.6 Co 0.2 Mn 0.2 O 2 Cathode with Improved Cycling Performance for Rechargeable Li-Ion Battery
journal, July 2016
- Wang, Hao; Ge, Wujie; Li, Wen
- ACS Applied Materials & Interfaces, Vol. 8, Issue 28
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
Paramecium-Like Iron Oxide Nanotubes as a Cost-Efficient Catalyst for Nonaqueous Lithium-Oxygen Batteries
journal, October 2017
- Zhang, Ruihan; Zhao, T. S.; Wu, Maochun
- Energy Technology, Vol. 6, Issue 2
A Li-S battery with ultrahigh cycling stability and enhanced rate capability based on novel ZnO yolk-shell sulfur host
journal, April 2021
- Zhang, Ruihan; Wu, Maochun; Fan, Xinzhuang
- Journal of Energy Chemistry, Vol. 55
Enhanced electrochemical performance of LiNi0.6Co0.2Mn0.2O2 cathode at high cutoff voltage by modifying electrode/electrolyte interface with lithium metasilicate
journal, August 2017
- Fu, Jiale; Mu, Daobin; Wu, Borong
- Electrochimica Acta, Vol. 246
Rechargeable alkaline zinc batteries: Progress and challenges
journal, October 2020
- Shang, Wenxu; Yu, Wentao; Liu, Yongfu
- Energy Storage Materials, Vol. 31
Recycling End-of-Life Electric Vehicle Lithium-Ion Batteries
journal, November 2019
- Chen, Mengyuan; Ma, Xiaotu; Chen, Bin
- Joule, Vol. 3, Issue 11
Electrical energy storage for transportation—approaching the limits of, and going beyond, lithium-ion batteries
journal, January 2012
- Thackeray, Michael M.; Wolverton, Christopher; Isaacs, Eric D.
- Energy & Environmental Science, Vol. 5, Issue 7
Understanding the role of trace amount of Fe incorporated in Ni-rich Li[Ni1-x-yCoxMny]O2 cathode material
journal, September 2020
- Park, Sanghyuk; Jo, Changheum; Kim, Hee Jae
- Journal of Alloys and Compounds, Vol. 835
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
Preparation of metal ion buffers for biological experimentation: A methods approach with emphasis on iron and zinc
journal, April 2002
- Aslamkhan, Amy G.; Aslamkhan, Abubakr; Ahearn, Gregory A.
- Journal of Experimental Zoology, Vol. 292, Issue 6
Structural, Electrochemical, and Thermal Properties of Nickel-Rich LiNi x Mn y Co z O 2 Materials
journal, November 2018
- Zhang, Ning; Li, Jing; Li, Hongyang
- Chemistry of Materials, Vol. 30, Issue 24
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
Role of impurity copper in Li-ion battery recycling to LiCoO2 cathode materials
journal, February 2020
- Peng, Chao; Lahtinen, Katja; Medina, Elena
- Journal of Power Sources, Vol. 450
Solvent-Free Manufacturing of Electrodes for Lithium-ion Batteries
journal, March 2016
- Ludwig, Brandon; Zheng, Zhangfeng; Shou, Wan
- Scientific Reports, Vol. 6, Issue 1