The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method

Zheng, Yadong; Azhari, Luqman; Meng, Zifei; Gao, Guanhui; Han, Yimo; Yang, Zhenzhen; Wang, Yan

doi:10.1021/acsami.2c12715

The Effects of Phosphate Impurity on Recovered LiNi_0.6Co_0.2Mn_0.2O₂ Cathode Material via a Hydrometallurgy Method

Journal Article · Wed Oct 19 00:00:00 EDT 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.2c12715· OSTI ID:2217030

^[1]; Azhari, Luqman ^[1]; Meng, Zifei ^[1]; Gao, Guanhui ^[2]; ^[2]; ^[3]; ^[1]

Worcester Polytechnic Institute, MA (United States)
Rice Univ., Houston, TX (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

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 LiNi_0.6Co_0.2Mn_0.2O₂ ("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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2217030

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 43 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (31)

Effect of precursor and synthesis temperature on the structural and electrochemical properties of Li(Ni0.5Co0.2Mn0.3)O2 Wu, Kuichen; Wang, Fei; Gao, Lulu Electrochimica Acta, Vol. 75 https://doi.org/10.1016/j.electacta.2012.05.035	journal	July 2012
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 Park, Sanghyuk; Kim, Duho; Ku, Heesuk Electrochimica Acta, Vol. 296 https://doi.org/10.1016/j.electacta.2018.11.001	journal	February 2019
Lithium sulfide-based cathode for lithium-ion/sulfur battery: Recent progress and challenges Kaiser, Mohammad Rejaul; Han, Zhaojun; Liang, Ji Energy Storage Materials, Vol. 19 https://doi.org/10.1016/j.ensm.2019.04.001	journal	May 2019
Recycling End-of-Life Electric Vehicle Lithium-Ion Batteries Chen, Mengyuan; Ma, Xiaotu; Chen, Bin Joule, Vol. 3, Issue 11 https://doi.org/10.1016/j.joule.2019.09.014	journal	November 2019
Minimization of the cation mixing in Li1+x(NMC)1−xO2 as cathode material Zhang, Xiaoyu; Jiang, W. J.; Mauger, A. Journal of Power Sources, Vol. 195, Issue 5 https://doi.org/10.1016/j.jpowsour.2009.09.029	journal	March 2010
A closed loop process for recycling spent lithium ion batteries Gratz, Eric; Sa, Qina; Apelian, Diran Journal of Power Sources, Vol. 262, p. 255-262 https://doi.org/10.1016/j.jpowsour.2014.03.126	journal	September 2014
A study on the impact of lithium-ion cell relaxation on electrochemical impedance spectroscopy Barai, Anup; Chouchelamane, Gael H.; Guo, Yue Journal of Power Sources, Vol. 280 https://doi.org/10.1016/j.jpowsour.2015.01.097	journal	April 2015
Surface engineering of LiNi0.8Mn0.1Co0.1O2 towards boosting lithium storage: Bimetallic oxides versus monometallic oxides Xu, Quan; Li, Xifei; Kheimeh Sari, Hirbod Maleki Nano Energy, Vol. 77 https://doi.org/10.1016/j.nanoen.2020.105034	journal	November 2020
Understanding fundamental effects of Cu impurity in different forms for recovered LiNi0.6Co0.2Mn0.2O2 cathode materials Zhang, Ruihan; Meng, Zifei; Ma, Xiaotu Nano Energy, Vol. 78 https://doi.org/10.1016/j.nanoen.2020.105214	journal	December 2020
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 Thompson, Dana; Hyde, Charlotte; Hartley, Jennifer M. Resources, Conservation and Recycling, Vol. 175 https://doi.org/10.1016/j.resconrec.2021.105741	journal	December 2021
Purification and Characterization of Reclaimed Electrolytes from Spent Lithium-Ion Batteries Liu, Yuanlong; Mu, Deying; Li, Ruhong The Journal of Physical Chemistry C, Vol. 121, Issue 8 https://doi.org/10.1021/acs.jpcc.6b12970	journal	February 2017
Revealing the Rate-Limiting Li-Ion Diffusion Pathway in Ultrathick Electrodes for Li-Ion Batteries Gao, Han; Wu, Qiang; Hu, Yixin The Journal of Physical Chemistry Letters, Vol. 9, Issue 17 https://doi.org/10.1021/acs.jpclett.8b02229	journal	August 2018
Valence Effects of Fe Impurity for Recovered LiNi _0.6 Co _0.2 Mn _0.2 O ₂ Cathode Materials Zhang, Ruihan; Zheng, Yadong; Vanaphuti, Panawan ACS Applied Energy Materials, Vol. 4, Issue 9 https://doi.org/10.1021/acsaem.1c02281	journal	September 2021
Stabilized Lithium, Manganese-Rich Layered Cathode Materials Enabled by Integrating Co-Doping and Nanocoating Vanaphuti, Panawan; Liu, Yangtao; Ma, Xiaotu ACS Applied Materials & Interfaces, Vol. 13, Issue 19 https://doi.org/10.1021/acsami.1c04718	journal	May 2021
Positive Role of Fluorine Impurity in Recovered LiNi_0.6Co_0.2Mn_0.2O₂ Cathode Materials Zheng, Yadong; Zhang, Ruihan; Vanaphuti, Panawan ACS Applied Materials & Interfaces, Vol. 13, Issue 48 https://doi.org/10.1021/acsami.1c17341	journal	November 2021
Copper Impurity Effects on LiNi _1/3 Mn _1/3 Co _1/3 O ₂ Cathode Material Sa, Qina; Heelan, Joseph A.; Lu, Yuan ACS Applied Materials & Interfaces, Vol. 7, Issue 37 https://doi.org/10.1021/acsami.5b04426	journal	September 2015
Enhancing the Electrocatalysis of LiNi _0.5 Co _0.2 Mn _0.3 O ₂ by Introducing Lithium Deficiency for Oxygen Evolution Reaction Huang, Di; Yu, Jiuling; Zhang, Zhengcheng ACS Applied Materials & Interfaces, Vol. 12, Issue 9 https://doi.org/10.1021/acsami.9b22438	journal	February 2020
Systematic Study of Al Impurity for NCM622 Cathode Materials Zhang, Ruihan; Zheng, Yadong; Yao, Zeyi ACS Sustainable Chemistry & Engineering, Vol. 8, Issue 26 https://doi.org/10.1021/acssuschemeng.0c02965	journal	June 2020
Unveiling the Influence of Carbon Impurity on Recovered NCM622 Cathode Material Zheng, Yadong; Zhang, Ruihan; Vanaphuti, Panawan ACS Sustainable Chemistry & Engineering, Vol. 9, Issue 17 https://doi.org/10.1021/acssuschemeng.1c01510	journal	April 2021
Recovery of Lithium, Iron, and Phosphorus from Spent LiFePO ₄ Batteries Using Stoichiometric Sulfuric Acid Leaching System Li, Huan; Xing, Shengzhou; Liu, Yu ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 9 https://doi.org/10.1021/acssuschemeng.7b01594	journal	August 2017
High Performance Cathode Recovery from Different Electric Vehicle Recycling Streams Zheng, Zhangfeng; Chen, Mengyuan; Wang, Qiang ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 11 https://doi.org/10.1021/acssuschemeng.8b02405	journal	September 2018
Batteries and fuel cells for emerging electric vehicle markets Cano, Zachary P.; Banham, Dustin; Ye, Siyu Nature Energy, Vol. 3, Issue 4 https://doi.org/10.1038/s41560-018-0108-1	journal	April 2018
Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease Cappello, Valentina; Marchetti, Laura; Parlanti, Paola Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/s41598-016-0001-8	journal	December 2016
Closed Loop Recycling of Electric Vehicle Batteries to Enable Ultra-high Quality Cathode Powder Chen, Mengyuan; Zheng, Zhangfeng; Wang, Qiang Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-018-38238-3	journal	February 2019
The impact of aluminum impurity on the regenerated lithium nickel cobalt manganese oxide cathode materials from spent LIBs Ren, Jie; Li, Ruhong; Liu, Yuanlong New Journal of Chemistry, Vol. 41, Issue 19 https://doi.org/10.1039/C7NJ01206C	journal	January 2017
The importance of design in lithium ion battery recycling – a critical review Thompson, Dana L.; Hartley, Jennifer M.; Lambert, Simon M. Green Chemistry, Vol. 22, Issue 22 https://doi.org/10.1039/D0GC02745F	journal	January 2020
Revealing the correlation between structural evolution and Li ⁺ diffusion kinetics of nickel-rich cathode materials in Li-ion batteries Hong, Chaoyu; Leng, Qianyi; Zhu, Jianping Journal of Materials Chemistry A, Vol. 8, Issue 17 https://doi.org/10.1039/D0TA00555J	journal	January 2020
A novel method to recycle mixed cathode materials for lithium ion batteries Zou, Haiyang; Gratz, Eric; Apelian, Diran Green Chemistry, Vol. 15, Issue 5 https://doi.org/10.1039/c3gc40182k	journal	January 2013
LiNi1/3Co1/3Mn1/3O2 hollow nano-micro hierarchical microspheres with enhanced performances as cathodes for lithium-ion batteries Li, Jili; Cao, Chuanbao; Xu, Xingyan Journal of Materials Chemistry A, Vol. 1, Issue 38 https://doi.org/10.1039/c3ta12375h	journal	January 2013
Cobalt in lithium-ion batteries Li, Matthew; Lu, Jun Science, Vol. 367, Issue 6481 https://doi.org/10.1126/science.aba9168	journal	February 2020
Progress and Status of Hydrometallurgical and Direct Recycling of Li-Ion Batteries and Beyond Larouche, François; Tedjar, Farouk; Amouzegar, Kamyab Materials, Vol. 13, Issue 3 https://doi.org/10.3390/ma13030801	journal	February 2020

Similar Records

Valence Effects of Fe Impurity for Recovered LiNi_0.6Co_0.2Mn_0.2O₂ Cathode Materials

Journal Article · Wed Sep 15 20:00:00 EDT 2021 · ACS Applied Energy Materials · OSTI ID:1840909

Positive Role of Fluorine Impurity in Recovered LiNi_0.6Co_0.2Mn_0.2O₂ Cathode Materials

Journal Article · Thu Nov 18 19:00:00 EST 2021 · ACS Applied Materials and Interfaces · OSTI ID:1838890

Related Subjects

25 ENERGY STORAGE
LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode
electrochemistry
hydrometallurgy recycling
lithium-ion batteries
phosphate impurity

The Effects of Phosphate Impurity on Recovered LiNi0.6Co0.2Mn0.2O2 Cathode Material via a Hydrometallurgy Method

Citation Formats

References (31)

Similar Records

Related Subjects

The Effects of Phosphate Impurity on Recovered LiNi_0.6Co_0.2Mn_0.2O₂ Cathode Material via a Hydrometallurgy Method