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Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion...
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Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion Batteries

A special issue of Metals (ISSN 2075-4701). This special issue belongs to the section "Extractive Metallurgy".

Deadline for manuscript submissions: closed (31 December 2022) | Viewed by 15722

Special Issue Editors

Prof. Dr. Alexandre Chagnes

E-Mail Website
Guest Editor
GeoRessources, Université de Lorraine, CNRS, 54000 Nancy, France
Interests: hydrometallurgy; lithium-ion battery; solvent extraction; recycling; circular economy
Special Issues, Collections and Topics in MDPI journals
Dr. Kerstin Forsberg

E-Mail Website
Guest Editor
Department of Chemical Engineering, KTH Royal Institute of Technology, Teknikringen 42, 100 44 Stockholm, Sweden
Interests: hydrometallurgy; crystallization; precipitation; recycling

Special Issue Information

Dear Colleagues,

The energy transition relies on the development of technologies that make it possible to produce energy in a sustainable manner from resources such as wind, sun, potential energy, etc. The energy produced as part of the energy transition is often intermittent, and it is, therefore, necessary to be able to store and restore it reversibly. Electric mobility is also a major contributor to reducing the impacts of human activity on the environment and the climate since it contributes to reducing greenhouse gas emissions. Lithium-ion batteries (LiBs) are at the heart of energy storage for stationary applications and for electric mobility (electric vehicles, EVs). They are now widely used in phones, laptops, portable tools, etc., and their increasing use in EVs is indisputable (about 3 million new electric cars were registered in 2020, including 1.4 million new registrations in Europe despite the pandemic). It is expected that this market (and the associated LiBs market) will continue to grow in the coming decades under the impulsion of the energy transition and since EV prices will reach parity with fossil-fuel powered autos in 2025.

Both primary and secondary resources are essential to meet the raw material demand for LiB production arising from the huge increase in electric vehicle production in the next decade. For example, cobalt, nickel, and lithium demand is forecasted to increase by 180%, 900%, and 1000% between 2019 and 2030, respectively.

This Special Issue aims at gathering outstanding works on the development of hydrometallurgical processes for a sustainable supply of metals for LiB production and the comprehension of the physical chemistry involved in their unit operations.

Prof. Dr. Alexandre Chagnes
Dr. Kerstin Forsberg
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Metals is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • hydrometallurgy
  • lithium-ion battery
  • solvent extraction
  • crystallization
  • recycling
  • mineral processing

Published Papers (5 papers)

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Research

23 pages, 8555 KiB  
Article
Influence of Pretreatment Strategy on the Crushing of Spent Lithium-Ion Batteries
by Denis Manuel Werner, Thomas Mütze and Urs Alexander Peuker
Metals 2022, 12(11), 1839; https://doi.org/10.3390/met12111839 - 28 Oct 2022
Cited by 6 | Viewed by 2899
Abstract
The rising production of lithium-ion batteries (LIBs) due to the introduction of electric mobility as well as stationary energy storage devices demands an efficient and sustainable waste management scheme for legislative, economic and ecologic reasons. One crucial part of the recycling of end-of-life [...] Read more.
The rising production of lithium-ion batteries (LIBs) due to the introduction of electric mobility as well as stationary energy storage devices demands an efficient and sustainable waste management scheme for legislative, economic and ecologic reasons. One crucial part of the recycling of end-of-life (EOL) LIBs is mechanical processes, which generate material fractions for the production of new batteries or further metallurgical refining. In the context of safe and efficient processing of electric vehicles’ LIBs, crushing is usually applied as a first process step to open at least the battery cell and liberate the cell components. However, the cell opening method used requires a specific pretreatment to overcome the LIB’s hazard potentials. Therefore, the dependence on pretreatment and crushing is investigated in this contribution. For this, the specific energy input for liberation is determined and compared for different recycling strategies with respect to dismantling depth and depollution temperatures. Furthermore, the respective crushing product is analyzed regarding granulometric properties, material composition, and liberation and decoating behaviour depending on the pretreatment and grid size of the crushing equipment. As a result, finer particles and components are generated with dried cells. Pyrolysis of cells as well as high dismantling depths do not allow to draw exact conclusions and predictions. Consequently, trends for a successful separation strategy of the subsequent classifying and sorting processes are revealed, and recommendations for the liberation of LIBs are derived. Full article
(This article belongs to the Special Issue Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion Batteries)
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16 pages, 4596 KiB  
Article
Direct Production of Ni–Co–Mn Mixtures for Cathode Precursors from Cobalt-Rich Lithium-Ion Battery Leachates by Solvent Extraction
by Niklas Jantunen, Sami Virolainen and Tuomo Sainio
Metals 2022, 12(9), 1445; https://doi.org/10.3390/met12091445 - 30 Aug 2022
Cited by 5 | Viewed by 2069
Abstract
A novel solvent extraction scheme was developed for the processing of Co-rich lithium-ion battery (LIB) leachate to a Ni–Co–Mn (NCM) sulfate mixture that can be directly used in the precursor synthesis of LIB cathodes. Conventional hydrometallurgical recycling of spent LIBs usually aims at [...] Read more.
A novel solvent extraction scheme was developed for the processing of Co-rich lithium-ion battery (LIB) leachate to a Ni–Co–Mn (NCM) sulfate mixture that can be directly used in the precursor synthesis of LIB cathodes. Conventional hydrometallurgical recycling of spent LIBs usually aims at separation of Li, Ni, Co, and Mn into pure fractions, which is simplified here. Operating pH and the number of extraction stages for each separation were evaluated from batch equilibrium experiments. Two continuous countercurrent extractions with bis(2-ethylhexyl) hydrogen phosphate (D2EHPA) and one with Cyanex 272 were studied in bench-scale mixer-settler equipment, and a Ni–Co–Mn solution with n(Ni):n(Co) = 14.16 and n(Ni):n(Mn) = 8.06 was obtained. The Ni:Co:Mn molar ratio in the NCM mixture can be adjusted to, for example, 8:1:1 using a Co-rich raffinate from the same process, and no additional transition metal salts are required for tuning the composition. Stripping raffinate containing 102.7 g L−1 Co at 99.8% relative purity was obtained from Cyanex 272 extraction. The main benefit of the process concept is that the solvent extraction separations can be operated with less stringent requirements than when producing pure metal salts. Full article
(This article belongs to the Special Issue Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion Batteries)
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19 pages, 7786 KiB  
Article
Phase Separation in a Novel Selective Lithium Extraction from Citrate Media with D2EHPA
by Tiaan Punt, Steven M. Bradshaw, Petrie Van Wyk and Guven Akdogan
Metals 2022, 12(9), 1400; https://doi.org/10.3390/met12091400 - 24 Aug 2022
Cited by 2 | Viewed by 1611
Abstract
Lithium-ion battery (LIB) recycling has received continued interest in recent years due to its benefits, which include reducing the environmental impact of spent LIBs and providing a secondary source of valuable metals, such as Li, Co, and Ni. This paper characterized the Li [...] Read more.
Lithium-ion battery (LIB) recycling has received continued interest in recent years due to its benefits, which include reducing the environmental impact of spent LIBs and providing a secondary source of valuable metals, such as Li, Co, and Ni. This paper characterized the Li separation with D2EHPA from citrate media as a function of pH and identified the optimal overall Li separation at a pH of 5.5. The Li separation was optimized at a pH of 5.5, with which it was concluded that 23 vol.% D2EHPA and an O/A ratio of 4 provided the best Li separation, for which 66.1% Li was extracted with 26.9% residual Mn, 6.8% Co, and 7.7% Ni in a single stage. The formation of a reversible hydrophobic third phase was identified during Li extraction at a pH of 5.5 or greater. Investigation of the third phase revealed that more than 99% of the Li, Co, and Ni were extracted to the third phase, while more than 69% of the Mn was extracted to the organic phase. STEM images of the third phase revealed a honeycomb-like structure, which was hypothesized to be a 2D mesoporous film caused by the insolubility of the organometallic complexes in the aqueous and organic phase. Full article
(This article belongs to the Special Issue Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion Batteries)
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15 pages, 3210 KiB  
Article
Solvent Extraction for Separation of 99.9% Pure Cobalt and Recovery of Li, Ni, Fe, Cu, Al from Spent LIBs
by Pratima Meshram, Sami Virolainen, Abhilash and Tuomo Sainio
Metals 2022, 12(6), 1056; https://doi.org/10.3390/met12061056 - 20 Jun 2022
Cited by 9 | Viewed by 4723
Abstract
In this work, hydrometallurgical recycling of metals from high-cobalt-content spent lithium-ion batteries (LIBs) from laptops was studied using precipitation and solvent extraction as alternative purification processes. Large amounts of cobalt (58% by weight), along with nickel (6.2%), manganese (3.06%) and lithium (6.09%) are [...] Read more.
In this work, hydrometallurgical recycling of metals from high-cobalt-content spent lithium-ion batteries (LIBs) from laptops was studied using precipitation and solvent extraction as alternative purification processes. Large amounts of cobalt (58% by weight), along with nickel (6.2%), manganese (3.06%) and lithium (6.09%) are present in LiCoO2 and Li2CoMn3O8 as prominent Co-rich phases of the electrode material. The pregnant leach solution (PLS) that was generated by leaching in the presence of 10% H2O2 using 50 g/L pulp density at 80 °C for 4 h contained 27.4 g/L Co, 3.21 g/L Ni, 1.59 g/L Mn and 3.60 g/L Li. The PLS was subjected to precipitation at various pH using 2 M NaOH but the purification performance was poor. To improve the separation of Mn and other impurities and in order to avoid the loss of cobalt and nickel, separation studies were carried out using a solvent extraction technique using di-(2-ethylhexyl) phosphoric acid (D2EHPA) and bis-(2,4,4-trimethylpentyl) phosphinic acid (Cyanex 272). Overall, this study examines the fundamentals of separating and synthesizing 99.9% pure Co sulfate from leach liquor of spent laptop LIBs with remarkably high cobalt content. Full article
(This article belongs to the Special Issue Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion Batteries)
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14 pages, 2829 KiB  
Article
Antisolvent Precipitation for Metal Recovery from Citric Acid Solution in Recycling of NMC Cathode Materials
by Wen Xuan, Alexandre Chagnes, Xiong Xiao, Richard T. Olsson and Kerstin Forsberg
Metals 2022, 12(4), 607; https://doi.org/10.3390/met12040607 - 31 Mar 2022
Cited by 15 | Viewed by 3342
Abstract
Lithium-ion batteries (LIBs) are widely used everywhere today, and their recycling is very important. This paper addresses the recovery of metals from NMC111 (LiNi1/3Mn1/3Co1/3O2) cathodic materials by leaching followed by antisolvent precipitation. Ultrasound-assisted leaching of [...] Read more.
Lithium-ion batteries (LIBs) are widely used everywhere today, and their recycling is very important. This paper addresses the recovery of metals from NMC111 (LiNi1/3Mn1/3Co1/3O2) cathodic materials by leaching followed by antisolvent precipitation. Ultrasound-assisted leaching of the cathodic material was performed in 1.5 mol L−1 citric acid at 50 °C and at a solid-to-liquid ratio of 20 g/L. Nickel(II), manganese(II) and cobalt(II) were precipitated from the leach liquor as citrates at 25 °C by adding an antisolvent (acetone or ethanol). No lithium(I) precipitation occurred under the experimental conditions, allowing for lithium separation. The precipitation efficiencies of manganese(II), cobalt(II) and nickel(II) decreased according to the order Mn > Co > Ni. The precipitation efficiency increased when a greater volume of antisolvent to the leachate was used. A smaller volume of acetone than ethanol was needed to reach the same precipitation efficiency in accordance with the difference in the dielectric constants of ethanol and acetone and their associated solubility constants. After adding two volumes of acetone into one volume of the leach liquor, 99.7% manganese, 97.0% cobalt and 86.9% nickel were recovered after 120 h, leaving lithium in the liquid phase. The metal citrates were converted into metal oxides by calcination at 900 °C. Full article
(This article belongs to the Special Issue Extractive Metallurgy for the Sustainable Supply of Metals in Lithium-Ion Batteries)
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