Electrodialysis: An effective methodology to purify the leachate of spent Li-ion batteries

Wang, Qiang; Fox, Robert V.; Shi, Meng; Snyder, Seth W.; Ilevbare, Gabriel O.; Ginosar, Daniel M.

doi:10.1016/j.seppur.2024.130430

Electrodialysis: An effective methodology to purify the leachate of spent Li-ion batteries

Journal Article · Fri Nov 08 00:00:00 EST 2024 · Separation and Purification Technology

DOI:https://doi.org/10.1016/j.seppur.2024.130430· OSTI ID:2499805

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Idaho National Laboratory (INL), Idaho Falls, ID (United States)
S.W. Scientific Investments LLC, Memphis, TN (United States)

The electrification of transportation and the transition of society towards low or net-zero carbon emissions has led to a skyrocketing global demand for Li-ion batteries. After a service life of three to ten years, Li-ion batteries have less than 80 % of their initial capacities and draw near to the end of their lives for practical utilization. Due to potential supply chain shortages and the value embodied in Li-ion batteries, it is imperative to recycle them, to recover the materials, and to improve the circularity and the sustinability of the industry. How to cost-effectively purify spent batteries while reducing time, energy, and waste emissions is a challenge faced by Li-ion battery recyclers. The first electrochemical membrane reactor reported in our group hasa high selectivity towards lower Cu²⁺, Al³⁺ and Fe³⁺ ions (<5 ppm) and retains >95% of the Ni²⁺, Co²⁺ and Mn²⁺ ions in the leachate. An advanced electrochemical membrane reactor was developed in this study. Further, not only does the new reactor have the same selectivity as the original reactor, but other advantages including a faster leachate processing rate (up to 10X faster). The advanced reactor can also directly generate acid at the anode side; eliminating the reactor restoration step. The prominent advantages that this electrodialysis technology has over chemical-precipitation methods include: (1) ion recovery efficiencies do not diminish after removing the impurities, Ni²⁺, Co²⁺ and Mn²⁺, even at a higher initial Ni²⁺ ion concentrations; in comparison, chemical precipitation has Ni²⁺, Co²⁺ and Mn²⁺ ion recovery efficiencies reduced significantly when the initial Ni²⁺, Co²⁺ and Mn²⁺ ion concentrations increase. (2) electrodialysis does not change the concentrations of Ni²⁺, Co²⁺ and Mn²⁺ ions significantly, but chemical precipitation could reduce Ni²⁺ and Co²⁺ ions to less than half of their initial values. Through electro-dialyzing the leachate, the H₂ evolution reaction mechanism was found to switch from the Volmer-acid Heyrovsky mechanism to the Volmer-alkaline Heyrovsky mechanism at a pH of around 3.7.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2499805

Report Number(s):: INL/JOU--24-78790-Rev000

Journal Information:: Separation and Purification Technology, Journal Name: Separation and Purification Technology Journal Issue: Part 1 Vol. 359; ISSN 1383-5866

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (23)

A Materials Perspective on Direct Recycling of Lithium‐Ion Batteries: Principles, Challenges and Opportunities Xu, Panpan; Tan, Darren H. S.; Jiao, Binglei Advanced Functional Materials, Vol. 33, Issue 14 https://doi.org/10.1002/adfm.202213168	journal	February 2023
The Hydrogen Evolution Reaction in Alkaline Solution: From Theory, Single Crystal Models, to Practical Electrocatalysts Zheng, Yao; Jiao, Yan; Vasileff, Anthony Angewandte Chemie International Edition, Vol. 57, Issue 26 https://doi.org/10.1002/anie.201710556	journal	May 2018
Reuse of LiCoO ₂ Electrodes Collected from Spent Li‐Ion Batteries after Electrochemical Re‐Lithiation of the Electrode Lahtinen, Katja; Rautama, Eeva‐Leena; Jiang, Hua ChemSusChem, Vol. 14, Issue 11 https://doi.org/10.1002/cssc.202100629	journal	May 2021
Nickel electrodeposition on different metallic substrates Gómez, E.; Pollina, R.; Vallés, E. Journal of Electroanalytical Chemistry, Vol. 386, Issue 1-2 https://doi.org/10.1016/0022-0728(95)03817-Z	journal	April 1995
Errors in atomic absorption spectrophotometric determination of Pb, Zn, Ni and Co in geologic materials Govett, G. J. S.; Whitehead, R. E. Journal of Geochemical Exploration, Vol. 2, Issue 2 https://doi.org/10.1016/0375-6742(73)90011-3	journal	September 1973
Nickel hydroxide electrodeposition from nickel nitrate solutions: mechanistic studies Jayashree, R. S.; Kamath, P. Vishnu Journal of Power Sources, Vol. 93, Issue 1-2 https://doi.org/10.1016/S0378-7753(00)00568-1	journal	February 2001
Application of saponified D2EHPA for the selective extraction of manganese from spend lithium-ion batteries Keller, A.; Hlawitschka, M. W.; Bart, H. -J. Chemical Engineering and Processing - Process Intensification, Vol. 171 https://doi.org/10.1016/j.cep.2021.108552	journal	January 2022
Extractive separation studies of manganese from spent lithium battery leachate using mixture of PC88A and Versatic 10 acid in kerosene Joo, Sung-Ho; Shin, Shun Myung; Shin, Dongju Hydrometallurgy, Vol. 156 https://doi.org/10.1016/j.hydromet.2015.06.002	journal	July 2015
Direct recycling of spent Li-ion batteries: Challenges and opportunities toward practical applications Wei, Gaolei; Liu, Yuxuan; Jiao, Binglei iScience, Vol. 26, Issue 9 https://doi.org/10.1016/j.isci.2023.107676	journal	September 2023
Understanding the effect of nonmetallic impurities in regenerated cathode materials for lithium-ion battery recycling by tracking down impurity elements Beak, Mincheol; Park, Jangho; Park, Sanghyuk Journal of Hazardous Materials, Vol. 425 https://doi.org/10.1016/j.jhazmat.2021.127907	journal	March 2022
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 promising approach for the recovery of high value-added metals from spent lithium-ion batteries Hu, Juntao; Zhang, Jialiang; Li, Hongxu Journal of Power Sources, Vol. 351 https://doi.org/10.1016/j.jpowsour.2017.03.093	journal	May 2017
Recovery of lithium from spent lithium-ion batteries using precipitation and electrodialysis techniques Song, Yunfeng; Zhao, Zhongwei Separation and Purification Technology, Vol. 206 https://doi.org/10.1016/j.seppur.2018.06.022	journal	November 2018
Solvent extraction of cobalt from spent lithium-ion batteries: Dynamic optimization of the number of extraction stages using factorial design of experiments and response surface methodology Vieceli, Nathália; Ottink, Thomas; Stopic, Srecko Separation and Purification Technology, Vol. 307 https://doi.org/10.1016/j.seppur.2022.122793	journal	February 2023
Electrification and decarbonization of spent Li-ion batteries purification by using an electrochemical membrane reactor Wang, Qiang; Diaz Aldana, Luis A.; Dufek, Eric J. Separation and Purification Technology, Vol. 307 https://doi.org/10.1016/j.seppur.2022.122828	journal	February 2023
Electrochemical process for electrode material of spent lithium ion batteries Prabaharan, G.; Barik, S. P.; Kumar, N. Waste Management, Vol. 68 https://doi.org/10.1016/j.wasman.2017.07.007	journal	October 2017
Recycling chains for lithium-ion batteries: A critical examination of current challenges, opportunities and process dependencies Windisch-Kern, Stefan; Gerold, Eva; Nigl, Thomas Waste Management, Vol. 138 https://doi.org/10.1016/j.wasman.2021.11.038	journal	February 2022
pH Effects on Hydrogen Evolution and Oxidation over Pt(111): Insights from First-Principles Lamoureux, Philomena Schlexer; Singh, Aayush R.; Chan, Karen ACS Catalysis, Vol. 9, Issue 7 https://doi.org/10.1021/acscatal.9b00268	journal	May 2019
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
Epitaxial Electrodeposition of Nickel on Pt(111) Electrode Chen, Wanchung; Yen, PoYu; Kuo, Yenchung The Journal of Physical Chemistry C, Vol. 116, Issue 40 https://doi.org/10.1021/jp3040677	journal	September 2012
Recycling lithium-ion batteries from electric vehicles Harper, Gavin; Sommerville, Roberto; Kendrick, Emma Nature, Vol. 575, Issue 7781 https://doi.org/10.1038/s41586-019-1682-5	journal	November 2019
Environmentally friendly recycling and effective repairing of cathode powders from spent LiFePO ₄ batteries Chen, Jiangping; Li, Qingwen; Song, Jishun Green Chemistry, Vol. 18, Issue 8 https://doi.org/10.1039/C5GC02650D	journal	January 2016
A NOVEL CLOSED LOOP PROCESS FOR RECYCLING SPENT Li-ION BATTERY CATHODE MATERIALS Jung, Joey Chung-Yen; Chow, Norman; Nacu, Anca International Journal of Green Energy, Vol. 18, Issue 15 https://doi.org/10.1080/15435075.2021.1914631	journal	July 2021

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