Removal of impurity Metals as Phosphates from Lithium-ion Battery leachates

Klaehn, John R.; Shi, Meng; Aldana Diaz, Luis A.; Molina Montes de Oca, Daniel Ernesto; Reich, Sabrina M.; Palasyuk, Olena; Repukaiti, Reyixiati; Lister, Tedd E.

doi:10.1016/j.hydromet.2023.106041

Removal of impurity Metals as Phosphates from Lithium-ion Battery leachates

Journal Article · Sat Feb 18 00:00:00 EST 2023 · Hydrometallurgy

DOI:https://doi.org/10.1016/j.hydromet.2023.106041· OSTI ID:1985484

^[1]; ^[1]; ^[1]; ^[1]; Reich, Sabrina M. ^[1]; Palasyuk, Olena ^[2]; Repukaiti, Reyixiati ^[1]; ^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Ames Laboratory (AMES), Ames, IA (United States)

Recovery of critical materials from end-of life (EOL) lithium-ion batteries (LIB) is gaining interest as demands for materials grows. Hydrometallurgical processes start with an intermediate product known as black mass which contains critical materials of interest (Co, Ni, Li, and graphite) as well as impurities such as Cu, Al, and Fe. These impurities are deleterious to downstream separation processes, as well as impact functionality of the final products. Here, these impurities effectively compete with most solvent extraction (SX) and metal recovery processes to diminish the overall yields of the desired materials. In this work, a process flowsheet is presented where a previously reported electrochemical leaching (ECL) process is followed by selective precipitation using diammonium hydrogen phosphate (DAP) to remove Cu, Al, and Fe from LIB leachate solutions. The electrochemical leach process removes Cu and produces a pH-adjusted leachate, ca. pH 2, without requiring an extra Cu extraction step. The addition of the precipitant DAP to leachate by slightly adjusting the pH to 3–4 at 45 °C, precipitates 95–99% of Al and Fe as their phosphates and the leachate retains >95% of Co, Ni and Li. After the filtration of phosphate impurities, the solution is ready for further processing, such as SX. As an unexpected result from the leachate processing, 20–30% of the Ni and Co co-crystalize as the double salt after cooling to room temperature, which could provide a shorter route to their recovery.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Buildings and Industry. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE

Grant/Contract Number:: AC07-05ID14517; AL-12-350-001

OSTI ID:: 1985484

Alternate ID(s):: OSTI ID: 1959398

Report Number(s):: INL/JOU-22-66863-Rev001; TRN: US2402680

Journal Information:: Hydrometallurgy, Vol. 217; ISSN 0304-386X

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (63)

A review of the processes and lab-scale techniques for the treatment of spent rechargeable NiMH batteries Innocenzi, Valentina; Ippolito, Nicolò Maria; De Michelis, Ida Journal of Power Sources, Vol. 362 https://doi.org/10.1016/j.jpowsour.2017.07.034	journal	September 2017
Solvent Extraction of Ni and Co from the Phosphoric Acid Leaching Solution of Laterite Ore by P204 and P507 Rao, Mingjun; Zhang, Tao; Li, Guanghui Metals, Vol. 10, Issue 4 https://doi.org/10.3390/met10040545	journal	April 2020
Precipitation of Iron and Aluminum Phosphates Directly from Aqueous Solution as a Function of Temperature from 50 to 200 °C Roncal-Herrero, Teresa; Rodríguez-Blanco, Juan Diego; Benning, Liane G. Crystal Growth & Design, Vol. 9, Issue 12 https://doi.org/10.1021/cg900654m	journal	October 2009
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
Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing wastewater Zhao, Chunlong; He, Mingming; Cao, Hongbin Frontiers of Chemical Science and Engineering, Vol. 14, Issue 4 https://doi.org/10.1007/s11705-019-1806-3	journal	June 2019
Addressing a Common Misconception: Ammonium Acetate as Neutral pH “Buffer” for Native Electrospray Mass Spectrometry Konermann, Lars Journal of The American Society for Mass Spectrometry, Vol. 28, Issue 9 https://doi.org/10.1007/s13361-017-1739-3	journal	July 2017
Transportation of electric vehicle lithium-ion batteries at end-of-life: A literature review Slattery, Margaret; Dunn, Jessica; Kendall, Alissa Resources, Conservation and Recycling, Vol. 174 https://doi.org/10.1016/j.resconrec.2021.105755	journal	November 2021
The interference of copper, iron and aluminum with hydrogen peroxide and its effects on reductive leaching of LiNi1/3Mn1/3Co1/3O2 Chernyaev, Alexander; Zou, Yuanmin; Wilson, Benjamin P. Separation and Purification Technology, Vol. 281 https://doi.org/10.1016/j.seppur.2021.119903	journal	January 2022
Phosphorus recovery and recycling – closing the loop Jupp, Andrew R.; Beijer, Steven; Narain, Ganesha C. Chemical Society Reviews, Vol. 50, Issue 1 https://doi.org/10.1039/D0CS01150A	journal	January 2021
From agricultural use of sewage sludge to nutrient extraction: A soil science outlook Kirchmann, Holger; Börjesson, Gunnar; Kätterer, Thomas Ambio, Vol. 46, Issue 2 https://doi.org/10.1007/s13280-016-0816-3	journal	September 2016
Recycling of mixed cathode lithium‐ion batteries for electric vehicles: Current status and future outlook Or, Tyler; Gourley, Storm W. D.; Kaliyappan, Karthikeyan Carbon Energy, Vol. 2, Issue 1 https://doi.org/10.1002/cey2.29	journal	March 2020
Growth and characterization of ammonium nickel-cobalt sulfate Tutton’s salt for UV light applications Ghosh, Santunu; Oliveira, Michelle; Pacheco, Tiago S. Journal of Crystal Growth, Vol. 487 https://doi.org/10.1016/j.jcrysgro.2018.02.027	journal	April 2018
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
A critical review on ammonium recovery from wastewater for sustainable wastewater management Ye, Yuanyao; Ngo, Huu Hao; Guo, Wenshan Bioresource Technology, Vol. 268 https://doi.org/10.1016/j.biortech.2018.07.111	journal	November 2018
Environmental and Economic Sustainability of Swine Wastewater Treatments Using Ammonia Stripping and Anaerobic Digestion: A Short Review Folino, Adele; Zema, Demetrio Antonio; Calabrò, Paolo S. Sustainability, Vol. 12, Issue 12 https://doi.org/10.3390/su12124971	journal	June 2020
Recovery of metals from spent lithium-ion battery leach solutions with a mixed solvent extractant system Pranolo, Y.; Zhang, W.; Cheng, C. Y. Hydrometallurgy, Vol. 102, Issue 1-4 https://doi.org/10.1016/j.hydromet.2010.01.007	journal	April 2010
The geology of aluminium phosphates and sulphates of the alunite group minerals: a review Dill, Harald G. Earth-Science Reviews, Vol. 53, Issue 1-2 https://doi.org/10.1016/S0012-8252(00)00035-0	journal	March 2001
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
On the design of crystallization-based separation processes: Review and extension Cisternas, Luis A.; Vásquez, Cristian M.; Swaney, Ross E. AIChE Journal, Vol. 52, Issue 5 https://doi.org/10.1002/aic.10768	journal	January 2006
Cobalt products from real waste fractions of end of life lithium ion batteries Pagnanelli, Francesca; Moscardini, Emanuela; Altimari, Pietro Waste Management, Vol. 51 https://doi.org/10.1016/j.wasman.2015.11.003	journal	May 2016
Solubility Product of Iron Phosphate1 Chang, S. C.; Jackson, M. L. Soil Science Society of America Journal, Vol. 21, Issue 3 https://doi.org/10.2136/sssaj1957.03615995002100030005x	journal	January 1957
Cobalt-nickel separation: the extraction of cobalt(II) and nickel(II) by Cyanex 301, Cyanex 302 and Cyanex 272 Tait, Brian K. Hydrometallurgy, Vol. 32, Issue 3 https://doi.org/10.1016/0304-386X(93)90047-H	journal	April 1993
Manganese metallurgy review. Part II: Manganese separation and recovery from solution Zhang, Wensheng; Cheng, Chu Yong Hydrometallurgy, Vol. 89, Issue 3-4 https://doi.org/10.1016/j.hydromet.2007.08.009	journal	December 2007
Development of a Novel Solvent Extraction Process to Recover Cobalt, Nickel, Manganese, and Lithium from Cathodic Materials of Spent Lithium-Ion Batteries Xuan, Wen; de Souza Braga, Antônio; Chagnes, Alexandre ACS Sustainable Chemistry & Engineering, Vol. 10, Issue 1 https://doi.org/10.1021/acssuschemeng.1c07109	journal	December 2021
Guano-related phosphate-rich minerals in European caves Audra, Philippe; De Waele, Jo International Journal of Speleology, Vol. 48, Issue 1 https://doi.org/10.5038/1827-806X.48.1.2252	journal	January 2019
On the Solubility Constant of Strengite Iuliano, Mauro; Ciavatta, Liberato; De Tommaso, Gaetano Soil Science Society of America Journal, Vol. 71, Issue 4 https://doi.org/10.2136/sssaj2006.0109	journal	January 2007
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
Remediation of contaminated land by formation of heavy metal phosphates Cotter-Howells, J.; Caporn, S. Applied Geochemistry, Vol. 11, Issue 1-2 https://doi.org/10.1016/0883-2927(95)00042-9	journal	January 1996
Recovery of metals from sulfate leach solutions of spent ternary lithium-ion batteries by precipitation with phosphate and solvent extraction with P507 Zhang, Kuifang; Liang, Helei; Zhong, Xiaocong Hydrometallurgy, Vol. 210 https://doi.org/10.1016/j.hydromet.2022.105861	journal	April 2022
Struvite formation and decomposition characteristics for ammonia and phosphorus recovery: A review of magnesium-ammonia-phosphate interactions Tansel, Berrin; Lunn, Griffin; Monje, Oscar Chemosphere, Vol. 194 https://doi.org/10.1016/j.chemosphere.2017.12.004	journal	March 2018
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
Infrared and Raman Spectroscopic Characterization of the Phosphate Mineral Leucophosphite K(Fe³⁺)₂(PO₄)₂(OH) · 2(H₂O) Frost, Ray L.; Xi, Yunfei; Scholz, Ricardo Spectroscopy Letters, Vol. 46, Issue 6 https://doi.org/10.1080/00387010.2012.733478	journal	August 2013
Removal of iron, aluminium, manganese and copper from leach solutions of lithium-ion battery waste using ion exchange Virolainen, Sami; Wesselborg, Tobias; Kaukinen, Arttu Hydrometallurgy, Vol. 202 https://doi.org/10.1016/j.hydromet.2021.105602	journal	June 2021
Recycling of spent lithium-ion battery cathode materials by ammoniacal leaching Ku, Heesuk; Jung, Yeojin; Jo, Minsang Journal of Hazardous Materials, Vol. 313 https://doi.org/10.1016/j.jhazmat.2016.03.062	journal	August 2016
Hydrometallurgical Processes for Recycling Spent Lithium-Ion Batteries: A Critical Review Yao, Yonglin; Zhu, Meiying; Zhao, Zhuo ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 11 https://doi.org/10.1021/acssuschemeng.8b03545	journal	September 2018
Evolution of Environmentally Friendly Strategies for Metal Extraction Shyam Sunder, Govind Sharma; Adhikari, Sandhya; Rohanifar, Ahmad Separations, Vol. 7, Issue 1 https://doi.org/10.3390/separations7010004	journal	January 2020
Comparison of iron(III) and aluminum in precipitation of phosphate from solution No authors listed Water Research, Vol. 10, Issue 10 https://doi.org/10.1016/0043-1354(76)90026-9	journal	January 1976
A Critical Review and Analysis on the Recycling of Spent Lithium-Ion Batteries Lv, Weiguang; Wang, Zhonghang; Cao, Hongbin ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 2 https://doi.org/10.1021/acssuschemeng.7b03811	journal	December 2017
A Review of Nickel, Copper, and Cobalt Recovery by Chelating Ion Exchange Resins from Mining Processes and Mining Tailings Botelho Junior, Amilton Barbosa; Dreisinger, David B.; Espinosa, Denise C. R. Mining, Metallurgy & Exploration, Vol. 36, Issue 1 https://doi.org/10.1007/s42461-018-0016-8	journal	November 2018
Solubility in the System Aluminum Phosphate-Phosphoric Acid-Water Brosheer, J. C.; Lenfesty, F. A.; Anderson, J. F. Journal of the American Chemical Society, Vol. 76, Issue 23 https://doi.org/10.1021/ja01652a016	journal	December 1954
Life cycle assessment of lithium‐ion battery recycling using pyrometallurgical technologies Rajaeifar, Mohammad Ali; Raugei, Marco; Steubing, Bernhard Journal of Industrial Ecology, Vol. 25, Issue 6 https://doi.org/10.1111/jiec.13157	journal	June 2021
Thermal treatment and ammoniacal leaching for the recovery of valuable metals from spent lithium-ion batteries Chen, Yongming; Liu, Nannan; Hu, Fang Waste Management, Vol. 75 https://doi.org/10.1016/j.wasman.2018.02.024	journal	May 2018
Technologies of lithium recycling from waste lithium ion batteries: a review Bae, Hyuntae; Kim, Youngsik Materials Advances https://doi.org/10.1039/D1MA00216C	journal	January 2021
E-pH Diagrams for the Li-Fe-P-H₂O System from 298 to 473 K: Thermodynamic Analysis and Application to the Wet Chemical Processes of the LiFePO₄ Cathode Material Jing, Qiankun; Zhang, Jialiang; Liu, Yubo The Journal of Physical Chemistry C, Vol. 123, Issue 23 https://doi.org/10.1021/acs.jpcc.9b02074	journal	May 2019
New progress of ammonia recovery during ammonia nitrogen removal from various wastewaters Xiang, Shuyu; Liu, Yuhuan; Zhang, Guangming World Journal of Microbiology and Biotechnology, Vol. 36, Issue 10 https://doi.org/10.1007/s11274-020-02921-3	journal	August 2020
Electrodialysis of Phosphates in Industrial-Grade Phosphoric Acid Machorro, J. J.; Olvera, J. C.; Larios, A. ISRN Electrochemistry, Vol. 2013 https://doi.org/10.1155/2013/865727	journal	December 2013
Process for the Recovery of Cobalt and Nickel from Sulphate Leach Liquors with Saponified Cyanex 272 and D2EHPA Reddy, B. Ramachandra; Park, Kyung Ho Separation Science and Technology, Vol. 42, Issue 9 https://doi.org/10.1080/01496390701310496	journal	June 2007
Growth and structural analysis of ammonium nickel cobalt sulfate hexahydrate crystals de Oliveira, Michelle; Ghosh, Santunu; Pacheco, Tiago S. Materials Research Express, Vol. 4, Issue 10 https://doi.org/10.1088/2053-1591/aa9194	journal	October 2017
Phosphate Recovery from Swine Wastewater by a Struvite Precipitation Electrolyzer Wang, Fang; Fu, Rao; Lv, Hang Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-45085-3	journal	June 2019
Precipitation of Phosphate from Ammonium Phosphate Solutions by Iron Oxide and Aluminum Hydroxide Taylor, A. W.; Gurney, E. L.; Frazier, A. W. Soil Science Society of America Journal, Vol. 29, Issue 3 https://doi.org/10.2136/sssaj1965.03615995002900030026x	journal	May 1965
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
Recycling of spent lithium-ion batteries in view of green chemistry Li, Yukun; Lv, Weiguang; Huang, Hanlin Green Chemistry, Vol. 23, Issue 17 https://doi.org/10.1039/D1GC01639C	journal	January 2021
On the dimorphy between the variscite and clinovariscite group: refined finestructural relationship of strengite and clinostrengite, Fe(PO4). 2H2O Taxer, K.; Bartl, H. Crystal Research and Technology, Vol. 39, Issue 12 https://doi.org/10.1002/crat.200410293	journal	December 2004
Use of Diammonium Phosphate to Reduce Heavy Metal Solubility and Transport in Smelter-Contaminated Soil McGowen, S. L.; Basta, N. T.; Brown, G. O. Journal of Environmental Quality, Vol. 30, Issue 2 https://doi.org/10.2134/jeq2001.302493x	journal	March 2001
Removal of heavy metal ions from water by using calcined phosphate as a new adsorbent Aklil, A.; Mouflih, M.; Sebti, S. Journal of Hazardous Materials, Vol. 112, Issue 3 https://doi.org/10.1016/j.jhazmat.2004.05.018	journal	August 2004
Targeted removal of aluminium and copper in Li-ion battery waste solutions by selective precipitation as valuable porous materials Cognet, Marine; Cambedouzou, Julien; Madhavi, Srinivasan Materials Letters, Vol. 268 https://doi.org/10.1016/j.matlet.2020.127564	journal	June 2020
Optimalisation of Magnesium Ammonium Phosphate Precipitation and its Applicability to the Removal of Ammonium Demeestere, K.; Smet, E.; Van Langenhove, H. Environmental Technology, Vol. 22, Issue 12 https://doi.org/10.1080/09593330.2001.11090876	journal	December 2001
Industrial Recycling of Lithium-Ion Batteries—A Critical Review of Metallurgical Process Routes Brückner, Lisa; Frank, Julia; Elwert, Tobias Metals, Vol. 10, Issue 8 https://doi.org/10.3390/met10081107	journal	August 2020
Leucophosphite K[Fe2(PO4)2(OH)(H2O)]·H2O: Hydrogen Bonding and Structural Relationships Dick, Stefan; Zeiske, Thomas Journal of Solid State Chemistry, Vol. 133, Issue 2 https://doi.org/10.1006/jssc.1997.7519	journal	November 1997
Processing of solutions containing nickel and ammonium sulphate through solvent extraction using PC-88A Reddy, B. R.; Parija, Chinmay; Sarma, P. V. R. Bhaskara Hydrometallurgy, Vol. 53, Issue 1 https://doi.org/10.1016/S0304-386X(99)00036-5	journal	July 1999
Recycling of End-of-Life Lithium Ion Batteries, Part I: Commercial Processes Pinegar, Haruka; Smith, York R. Journal of Sustainable Metallurgy, Vol. 5, Issue 3 https://doi.org/10.1007/s40831-019-00235-9	journal	July 2019
Spent lithium-ion battery recycling – Reductive ammonia leaching of metals from cathode scrap by sodium sulphite Zheng, Xiaohong; Gao, Wenfang; Zhang, Xihua Waste Management, Vol. 60 https://doi.org/10.1016/j.wasman.2016.12.007	journal	February 2017
Effect of Na from the leachate of spent Li-ion batteries on the properties of resynthesized Li-ion battery cathodes Beak, Mincheol; Park, Sanghyuk; Kim, Sangjun Journal of Alloys and Compounds, Vol. 873 https://doi.org/10.1016/j.jallcom.2021.159808	journal	August 2021

Similar Records

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 · OSTI ID:2205582

Wang, Qiang; Aldana, Luis A. Diaz; Dufek, Eric J.; +3 more

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 · OSTI ID:2499805

Wang, Qiang; Fox, Robert V.; Shi, Meng; +3 more

Separation of cobalt, nickel, and manganese in leach solutions of waste lithium-ion batteries using Dowex M4195 ion exchange resin

Journal Article · Tue Oct 05 00:00:00 EDT 2021 · Hydrometallurgy · OSTI ID:1897968

Strauss, Mark L.; Diaz Aldana, Luis A.; McNally, Joshua S.; +2 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Precipitation
Lithium ion battery
Impurity metals
Phosphate
Leachate
Critical materials
Diammonium phosphate
Metal impurities removal
Lithium-ion battery leachate
Aluminum phosphate
Iron phosphate
Double salts

Removal of impurity Metals as Phosphates from Lithium-ion Battery leachates

Citation Formats

References (63)

Similar Records

Related Subjects