Electrification and decarbonization of spent Li-ion batteries purification by using an electrochemical membrane reactor

Wang, Qiang; Aldana, Luis A. Diaz; Dufek, Eric J.; Ginosar, Daniel M.; Klaehn, John R.; Shi, Meng

doi:10.1016/j.seppur.2022.122828

Electrification and decarbonization of spent Li-ion batteries purification by using an electrochemical membrane reactor

Journal Article · Fri Dec 02 00:00:00 EST 2022 · Separation and Purification Technology

DOI:https://doi.org/10.1016/j.seppur.2022.122828· OSTI ID:2205582

Wang, Qiang ^[1]; Aldana, Luis A. Diaz ^[1]; Dufek, Eric J. ^[1]; Ginosar, Daniel M. ^[1]; Klaehn, John R. ^[1]; Shi, Meng ^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)

The expanding electric vehicle market brings with it exponential growth in the use of lithium (Li)-ion batteries (LIB) for which a wave of spent LIB is expected to come within the next 5 to 10 years. Due to the economic and strategic value imbedded within the metals contained in LIB, different recycling technologies, including hydrometallurgy, pyrometallurgy and direct recycling, are under development. Being different from previous hydrometallurgical methods, which may have high chemical consumption and negative environmental impact, an electrochemical membrane reactor is designed and validated for the first time, to electrify and decarbonize the impurity removal process. This reactor electroplates copper (Cu) and electrochemically precipitates aluminum (Al) and iron (Fe) from simulated spent LIB leachates, by consuming only air, water, and electricity, and the impurities are reduced to <1 ppm. The purified leachate maintains 99.5 % of the nickel (Ni), 95.4 % of the cobalt (Co) and 99.14 % of manganese (Mn) from the original leachate solution, and then can be directly applied for cathode precursor synthesis. Additionally, the purification process doesn’t introduce extra impurity, and the reactor restoration process generates valuable by-product hydro sulfate (H2SO4). This electrochemical process can reduce the cost, because of the much less chemical consumption and the valuable by-product generation, and mitigates the waste emissions, because of no extra impurity introduced and no greenhouse gas (GHG) produced. In conclusion, the chemical precipitation method uses significant amount of NaOH, which induced GHG emission during the manufacturing process.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2205582

Alternate ID(s):: OSTI ID: 1961298

Report Number(s):: INL/JOU--21-64236-Rev001

Journal Information:: Separation and Purification Technology, Journal Name: Separation and Purification Technology Vol. 307; ISSN 1383-5866

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (30)

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
Comparision of Different Reductants in Leaching of Spent Lithium Ion Batteries Meshram, Pratima; Pandey, Banshi Dhar JOM, Vol. 68, Issue 10, p. 2613-2623 https://doi.org/10.1007/s11837-016-2032-9	journal	July 2016
Cobalt oxide preparation from waste LiCoO2 by electrochemical–hydrothermal method Myoung, Jinsik; Jung, Youngwoo; Lee, Jaeyoung Journal of Power Sources, Vol. 112, Issue 2 https://doi.org/10.1016/S0378-7753(02)00459-7	journal	November 2002
Acid leaching of mixed spent Li-ion batteries Nayl, A. A.; Elkhashab, R. A.; Badawy, Sayed M. Arabian Journal of Chemistry, Vol. 10 https://doi.org/10.1016/j.arabjc.2014.04.001	journal	May 2017
Electrochemical methods for sustainable recovery of lithium from natural brines and battery recycling Calvo, Ernesto Julio Current Opinion in Electrochemistry, Vol. 15 https://doi.org/10.1016/j.coelec.2019.04.010	journal	June 2019
Influence of the proton transport on the ORR kinetics and on the H2O2 escape in three-dimensionally ordered electrodes Rouhet, M.; Bozdech, S.; Bonnefont, A. Electrochemistry Communications, Vol. 33 https://doi.org/10.1016/j.elecom.2013.05.003	journal	August 2013
Renovation of LiCoO 2 with outstanding cycling stability by thermal treatment with Li 2 CO 3 from spent Li-ion batteries Chen, Shi; He, Tao; Lu, Yun Journal of Energy Storage, Vol. 8 https://doi.org/10.1016/j.est.2016.10.008	journal	November 2016
Leaching and separation of Co and Mn from electrode materials of spent lithium-ion batteries using hydrochloric acid: Laboratory and pilot scale study Barik, S. P.; Prabaharan, G.; Kumar, L. Journal of Cleaner Production, Vol. 147 https://doi.org/10.1016/j.jclepro.2017.01.095	journal	March 2017
Lithium-Ion Battery Supply Chain Considerations: Analysis of Potential Bottlenecks in Critical Metals Olivetti, Elsa A.; Ceder, Gerbrand; Gaustad, Gabrielle G. Joule, Vol. 1, Issue 2 https://doi.org/10.1016/j.joule.2017.08.019	journal	October 2017
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
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 review on the growing concern and potential management strategies of waste lithium-ion batteries Winslow, Kevin M.; Laux, Steven J.; Townsend, Timothy G. Resources, Conservation and Recycling, Vol. 129 https://doi.org/10.1016/j.resconrec.2017.11.001	journal	February 2018
Electrochemical-assisted leaching of active materials from lithium ion batteries Diaz, Luis A.; Strauss, Mark L.; Adhikari, Birendra Resources, Conservation and Recycling, Vol. 161 https://doi.org/10.1016/j.resconrec.2020.104900	journal	October 2020
Separation of lithium, nickel, manganese, and cobalt from waste lithium-ion batteries using electrodialysis Chan, Ka Ho; Malik, Monu; Azimi, Gisele Resources, Conservation and Recycling, Vol. 178 https://doi.org/10.1016/j.resconrec.2021.106076	journal	March 2022
The multiplex network structure of global cobalt industry chain Shi, Qing; Sun, Xiaoqi; Xu, Man Resources Policy, Vol. 76 https://doi.org/10.1016/j.resourpol.2022.102555	journal	June 2022
Hydrometallurgical recovery of metal values from sulfuric acid leaching liquor of spent lithium-ion batteries Chen, Xiangping; Chen, Yongbin; Zhou, Tao Waste Management, Vol. 38 https://doi.org/10.1016/j.wasman.2014.12.023	journal	April 2015
Reaction Mechanism for Oxygen Reduction on Platinum: Existence of a Fast Initial Chemical Step and a Soluble Species Different from H ₂ O ₂ Gómez-Marín, Ana; Feliu, Juan; Edson, Ticianelli ACS Catalysis, Vol. 8, Issue 9 https://doi.org/10.1021/acscatal.8b01291	journal	July 2018
Oxygen Reduction on Platinum Surfaces in Acid Media: Experimental Evidence of a CECE/DISP Initial Reaction Path Gómez-Marín, Ana M.; Feliu, Juan M.; Ticianelli, Edson ACS Catalysis, Vol. 9, Issue 3 https://doi.org/10.1021/acscatal.8b03351	journal	January 2019
A Green and Cost-Effective Method for Production of LiOH from Spent LiFePO₄ Li, Zheng; He, Lihua; Zhu, Yunfei ACS Sustainable Chemistry & Engineering, Vol. 8, Issue 42 https://doi.org/10.1021/acssuschemeng.0c04960	journal	September 2020
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
Sustainable and Facile Method for the Selective Recovery of Lithium from Cathode Scrap of Spent LiFePO₄ Batteries Zhang, Jialiang; Hu, Juntao; Liu, Yubo ACS Sustainable Chemistry & Engineering, Vol. 7, Issue 6 https://doi.org/10.1021/acssuschemeng.9b00404	journal	February 2019
Deep eutectic solvents for cathode recycling of Li-ion batteries Tran, Mai K.; Rodrigues, Marco-Tulio F.; Kato, Keiko Nature Energy, Vol. 4, Issue 4 https://doi.org/10.1038/s41560-019-0368-4	journal	April 2019
Examining different recycling processes for lithium-ion batteries Ciez, Rebecca E.; Whitacre, J. F. Nature Sustainability, Vol. 2, Issue 2 https://doi.org/10.1038/s41893-019-0222-5	journal	February 2019
Direct regeneration of cathode materials from spent lithium iron phosphate batteries using a solid phase sintering method Song, X.; Hu, T.; Liang, C. RSC Advances, Vol. 7, Issue 8 https://doi.org/10.1039/C6RA27210J	journal	January 2017
Impurity removal with highly selective and efficient methods and the recycling of transition metals from spent lithium-ion batteries Peng, Fangwei; Mu, Deying; Li, Ruhong RSC Advances, Vol. 9, Issue 38 https://doi.org/10.1039/C9RA02331C	journal	January 2019
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
Electrodialysis of a Lithium Sulphate Solution: An Experimental Investigation Kang, Bolin; Kang, Dongxin; Jung, Joey Chung-Yen Joey Journal of The Electrochemical Society, Vol. 169, Issue 6 https://doi.org/10.1149/1945-7111/ac76e6	journal	June 2022
Current Li-Ion Battery Technologies in Electric Vehicles and Opportunities for Advancements Miao, Yu; Hynan, Patrick; von Jouanne, Annette Energies, Vol. 12, Issue 6 https://doi.org/10.3390/en12061074	journal	March 2019
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
Application of Electrodialysis for the Selective Lithium Extraction Towards Cobalt, Nickel and Manganese from Leach Solutions Containing High Divalent Cations/Li Ratio Gmar, Soumaya; Chagnes, Alexandre; Lutin, Florence Recycling, Vol. 7, Issue 2 https://doi.org/10.3390/recycling7020014	journal	March 2022

Similar Records

Unraveling the nature of sulfide ions in hydrometallurgical recycling of NCM622 cathode material

Journal Article · Thu Feb 09 19:00:00 EST 2023 · Energy Storage Materials · OSTI ID:2349074

Recovery of Rare Earth Elements from Bioleachates by Precipitation

Technical Report · Tue Aug 25 20:00:00 EDT 2020 · OSTI ID:1668825

Systematic Study of Al Impurity for NCM622 Cathode Materials

Journal Article · Tue Jun 09 20:00:00 EDT 2020 · ACS Sustainable Chemistry & Engineering · OSTI ID:1650013

Related Subjects

25 ENERGY STORAGE
Critical materials
Electrochemical membrane reactor
Electrodialysis
Li ion battery
Li-ion batteries recycling
critical material
electrochemical membrane reactor
hydro-metallurgy
recycling

Electrification and decarbonization of spent Li-ion batteries purification by using an electrochemical membrane reactor

Citation Formats

References (30)

Similar Records

Related Subjects