The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method
Abstract
From portable electronics to electric vehicles, lithium-ion batteries have been deeply integrated into our daily life and industrial fields for a few decades. The booming field of battery manufacturing could lead to shortages in resources and massive accumulation of battery waste, hindering sustainable development. Therefore, hydrometallurgy-based approaches have been widely used in industrial recycling to recover cathode materials due to their high efficiency and throughput. Further, impurities have always been a great challenge for hydrometallurgical recycling, introducing challenges to maintain the consistency of product quality because of potential unintended effects caused by impurities. Herein, after comprehensive investigation, we first report the impacts of phosphate impurity on a recycled LiNi0.6Co0.2Mn0.2O2 ("NCM622") cathode via a hydrometallurgy method. We demonstrate that a passivation layer of Li3PO4 is formed at grain boundaries during sintering, which significantly raises the activation barrier and hinders lithium diffusion. In addition, the distinct degradation of cathode electrochemical properties is observed from poor particle morphology and high cation mixing as a result of phosphate impurity. Cathode powders with 1 at. % phosphate impurity retain a capacity of 146 mAh/g after 100 cycles at 0.33C, 6% less than that of a virgin cathode. Furthermore, cathodes with higher phosphate concentrations perform evenmore »
- Authors:
-
- Worcester Polytechnic Institute, MA (United States)
- Rice Univ., Houston, TX (United States)
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
- OSTI Identifier:
- 2217030
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 43; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; lithium-ion batteries; hydrometallurgy recycling; LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode; phosphate impurity; electrochemistry
Citation Formats
Zheng, Yadong, Azhari, Luqman, Meng, Zifei, Gao, Guanhui, Han, Yimo, Yang, Zhenzhen, and Wang, Yan. The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method. United States: N. p., 2022.
Web. doi:10.1021/acsami.2c12715.
Zheng, Yadong, Azhari, Luqman, Meng, Zifei, Gao, Guanhui, Han, Yimo, Yang, Zhenzhen, & Wang, Yan. The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method. United States. https://doi.org/10.1021/acsami.2c12715
Zheng, Yadong, Azhari, Luqman, Meng, Zifei, Gao, Guanhui, Han, Yimo, Yang, Zhenzhen, and Wang, Yan. Wed .
"The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method". United States. https://doi.org/10.1021/acsami.2c12715. https://www.osti.gov/servlets/purl/2217030.
@article{osti_2217030,
title = {The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method},
author = {Zheng, Yadong and Azhari, Luqman and Meng, Zifei and Gao, Guanhui and Han, Yimo and Yang, Zhenzhen and Wang, Yan},
abstractNote = {From portable electronics to electric vehicles, lithium-ion batteries have been deeply integrated into our daily life and industrial fields for a few decades. The booming field of battery manufacturing could lead to shortages in resources and massive accumulation of battery waste, hindering sustainable development. Therefore, hydrometallurgy-based approaches have been widely used in industrial recycling to recover cathode materials due to their high efficiency and throughput. Further, impurities have always been a great challenge for hydrometallurgical recycling, introducing challenges to maintain the consistency of product quality because of potential unintended effects caused by impurities. Herein, after comprehensive investigation, we first report the impacts of phosphate impurity on a recycled LiNi0.6Co0.2Mn0.2O2 ("NCM622") cathode via a hydrometallurgy method. We demonstrate that a passivation layer of Li3PO4 is formed at grain boundaries during sintering, which significantly raises the activation barrier and hinders lithium diffusion. In addition, the distinct degradation of cathode electrochemical properties is observed from poor particle morphology and high cation mixing as a result of phosphate impurity. Cathode powders with 1 at. % phosphate impurity retain a capacity of 146 mAh/g after 100 cycles at 0.33C, 6% less than that of a virgin cathode. Furthermore, cathodes with higher phosphate concentrations perform even worse in electrochemical tests. Therefore, phosphate impurities are detrimental to the hydrometallurgical recycling of NCM cathode materials and need to be excluded from the recycling process.},
doi = {10.1021/acsami.2c12715},
journal = {ACS Applied Materials and Interfaces},
number = 43,
volume = 14,
place = {United States},
year = {Wed Oct 19 00:00:00 EDT 2022},
month = {Wed Oct 19 00:00:00 EDT 2022}
}
Works referenced in this record:
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
The importance of design in lithium ion battery recycling – a critical review
journal, January 2020
- Thompson, Dana L.; Hartley, Jennifer M.; Lambert, Simon M.
- Green Chemistry, Vol. 22, Issue 22
Batteries and fuel cells for emerging electric vehicle markets
journal, April 2018
- Cano, Zachary P.; Banham, Dustin; Ye, Siyu
- Nature Energy, Vol. 3, Issue 4
Surface engineering of LiNi0.8Mn0.1Co0.1O2 towards boosting lithium storage: Bimetallic oxides versus monometallic oxides
journal, November 2020
- Xu, Quan; Li, Xifei; Kheimeh Sari, Hirbod Maleki
- Nano Energy, Vol. 77
Recovery of Lithium, Iron, and Phosphorus from Spent LiFePO 4 Batteries Using Stoichiometric Sulfuric Acid Leaching System
journal, August 2017
- Li, Huan; Xing, Shengzhou; Liu, Yu
- ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 9
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
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
A study on the impact of lithium-ion cell relaxation on electrochemical impedance spectroscopy
journal, April 2015
- Barai, Anup; Chouchelamane, Gael H.; Guo, Yue
- Journal of Power Sources, Vol. 280
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
Revealing the correlation between structural evolution and Li + diffusion kinetics of nickel-rich cathode materials in Li-ion batteries
journal, January 2020
- Hong, Chaoyu; Leng, Qianyi; Zhu, Jianping
- Journal of Materials Chemistry A, Vol. 8, Issue 17
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
Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease
journal, December 2016
- Cappello, Valentina; Marchetti, Laura; Parlanti, Paola
- Scientific Reports, Vol. 6, Issue 1
Cobalt in lithium-ion batteries
journal, February 2020
- Li, Matthew; Lu, Jun
- Science, Vol. 367, Issue 6481
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
Lithium sulfide-based cathode for lithium-ion/sulfur battery: Recent progress and challenges
journal, May 2019
- Kaiser, Mohammad Rejaul; Han, Zhaojun; Liang, Ji
- Energy Storage Materials, Vol. 19
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
Valence Effects of Fe Impurity for Recovered LiNi 0.6 Co 0.2 Mn 0.2 O 2 Cathode Materials
journal, September 2021
- Zhang, Ruihan; Zheng, Yadong; Vanaphuti, Panawan
- ACS Applied Energy Materials, Vol. 4, Issue 9
Revealing the Rate-Limiting Li-Ion Diffusion Pathway in Ultrathick Electrodes for Li-Ion Batteries
journal, August 2018
- Gao, Han; Wu, Qiang; Hu, Yixin
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 17
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
Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material
journal, April 2021
- Zheng, Yadong; Zhang, Ruihan; Vanaphuti, Panawan
- ACS Sustainable Chemistry & Engineering, Vol. 9, Issue 17
To shred or not to shred: A comparative techno-economic assessment of lithium ion battery hydrometallurgical recycling retaining value and improving circularity in LIB supply chains
journal, December 2021
- Thompson, Dana; Hyde, Charlotte; Hartley, Jennifer M.
- Resources, Conservation and Recycling, Vol. 175
Recycling End-of-Life Electric Vehicle Lithium-Ion Batteries
journal, November 2019
- Chen, Mengyuan; Ma, Xiaotu; Chen, Bin
- Joule, Vol. 3, Issue 11
The impact of aluminum impurity on the regenerated lithium nickel cobalt manganese oxide cathode materials from spent LIBs
journal, January 2017
- Ren, Jie; Li, Ruhong; Liu, Yuanlong
- New Journal of Chemistry, Vol. 41, Issue 19
Progress and Status of Hydrometallurgical and Direct Recycling of Li-Ion Batteries and Beyond
journal, February 2020
- Larouche, François; Tedjar, Farouk; Amouzegar, Kamyab
- Materials, Vol. 13, Issue 3
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
Purification and Characterization of Reclaimed Electrolytes from Spent Lithium-Ion Batteries
journal, February 2017
- Liu, Yuanlong; Mu, Deying; Li, Ruhong
- The Journal of Physical Chemistry C, Vol. 121, Issue 8
Enhancing the Electrocatalysis of LiNi 0.5 Co 0.2 Mn 0.3 O 2 by Introducing Lithium Deficiency for Oxygen Evolution Reaction
journal, February 2020
- Huang, Di; Yu, Jiuling; Zhang, Zhengcheng
- ACS Applied Materials & Interfaces, Vol. 12, Issue 9
Stabilized Lithium, Manganese-Rich Layered Cathode Materials Enabled by Integrating Co-Doping and Nanocoating
journal, May 2021
- Vanaphuti, Panawan; Liu, Yangtao; Ma, Xiaotu
- ACS Applied Materials & Interfaces, Vol. 13, Issue 19
Positive Role of Fluorine Impurity in Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Materials
journal, November 2021
- Zheng, Yadong; Zhang, Ruihan; Vanaphuti, Panawan
- ACS Applied Materials & Interfaces, Vol. 13, Issue 48
Minimization of the cation mixing in Li1+x(NMC)1−xO2 as cathode material
journal, March 2010
- Zhang, Xiaoyu; Jiang, W. J.; Mauger, A.
- Journal of Power Sources, Vol. 195, Issue 5