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Special Issue "New Science Based Concepts for Increased Efficiency in Battery Recycling 2023"

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

Deadline for manuscript submissions: 30 September 2023 | Viewed by 14500

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Special Issue Editor

Prof. Dr. Bernd Friedrich

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Guest Editor

IME Process Metallurgy and Metal Recycling Department, RWTH Aachen University, 52072 Aachen, Germany
Interests: process technology; metals; recycling; purification; alloying; WEEE; spent batteries; critical materials; circular economy
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

There is no doubt that e-mobility will become a tremendous driving force for our future life. High demand for advanced materials in the batteries as well as political pressures in terms of collection and recycling rates raise the need for an extensive recovery of critical elements and a more sustainable use of raw materials. This Special Issue aims to make significant progress in designing innovative processes and understanding related mechanisms in the context of battery recycling. Although we expect the majority of papers to address the latest scientific achievements in the area of lithium-based systems, the entire range from lead, to nickel–metal–hydride, to high-temperature vanadium sodium cells is covered by this compilation. Of special interest are concepts for future post-Li-systems including all solid-state cell designs. We are not focusing on consumer behavior, collection, legal, and regulation issues and market development. Papers dealing with automized disassambly/dismantling, sensor-based sorting, new concepts for comminution and classification, thermal conditioning, innovations in hydro- and pyrometallurgical processing, safety aspects regarding recycling processes, post-mortem analysis with regards to cell chemistry changes, as well as mass flow analysis and optimization models for recycling efficiency are welcome.

The idea of a circular economy is the point of origin for contributions, aiming at minimizing of waste streams and promoting re-use/recirculation of components, functional materials as well as elements. In order to minimize material losses and energy consumption, this Issue explores concepts for optimization concerning the interfaces between mechanical and thermal pre-treatments with metallurgical processes. Considering both principle aspects of circular economy and material design, the topics of special interest are those concerning recovery and re-use of critical metals like lithium, since their importance for technological applications often goes along with a lack of supply on the world market.

This Special Issue follows the 2020 issue, which can be found under
https://www.mdpi.com/journal/metals/special_issues/battery_recycling

Prof. Dr. Bernd Friedrich
Guest Editor

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 2000 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

battery recycling
resource efficiency
circular economy
recovery
critical metals
waste minimization

Published Papers (7 papers)

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Research

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Open AccessArticle

Acid Leaching of Al- and Ta-Substituted Li₇La₃Zr₂O₁₂ (LLZO) Solid Electrolyte

and

Metals 2023, 13(5), 834; https://doi.org/10.3390/met13050834 - 24 Apr 2023

Viewed by 599

Abstract

Solid-state batteries (SSBs) are promising next-generation batteries due to their potential for achieving high energy densities and improved safety compared to conventional lithium-ion batteries (LIBs) with a flammable liquid electrolyte. Despite their huge market potential, very few studies have investigated SSB recycling processes to recover and reuse critical raw metals for a circular economy. For conventional LIBs, hydrometallurgical recycling has been proven to be able to produce high-quality products, with leaching being the first unit operation. Therefore, it is essential to establish a fundamental understanding of the leaching behavior of solid electrolytes as the key component of SSBs with different lixiviants. This work investigates the leaching of the most promising Al- and Ta-substituted Li₇La₃Zr₂O₁₂ (LLZO) solid electrolytes in mineral acids (H₂SO₄ and HCl), organic acids (formic, acetic, oxalic, and citric acid), and water. The leaching experiments were conducted using actual LLZO production waste in 1 M of acid at 1:20 S/L ratio at 25 °C for 24 h. The results showed that strong acids, such as H₂SO₄, almost completely dissolved LLZO. Encouraging selective leaching properties were observed with oxalic acid and water. This fundamental knowledge of LLZO leaching behavior will provide the basis for future optimization studies to develop innovative hydrometallurgical SSB recycling processes. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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Open AccessArticle

Evaluation of the Influence Exerted by Increased Silicon Contents on the Leaching Behavior of NMC-Based Black Mass

Eva Gerold

Reinhard Lerchbammer

and

Helmut Antrekowitsch

Metals 2023, 13(4), 785; https://doi.org/10.3390/met13040785 - 17 Apr 2023

Viewed by 423

Abstract

The further development of lithium-ion batteries leads to an improvement in power densities as well as safety and thus requires an optimization of the materials used. For this purpose, among other approaches, the anode materials are doped with silicon oxide or metallic silicon is used as the anode. However, silicon is a semimetal and is known to lead to the formation of jelly-like fluids in hydrometallurgical processes under certain conditions. This publication evaluates which parameters are responsible for this viscosity change in the leaching solutions during the recycling of lithium-ion batteries and examines the corresponding reaction mechanism behind this phenomenon. Furthermore, the leaching efficiency for the valuable metals nickel, cobalt, lithium and manganese is evaluated and the influence of different silicon contents in the solution is investigated. It could be shown that, especially the simultaneous presence of H₂SO₄, H₂O₂ and Si or SiO_2, lead to a significant viscosity increase due to the formation of metasilicic acid and, accordingly, the leaching efficiencies of the valuable metals are negatively influenced. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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Open AccessArticle

Selective Sulfation Roasting for Cobalt and Lithium Extraction from Industrial LCO-Rich Spent Black Mass

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Metals 2023, 13(2), 358; https://doi.org/10.3390/met13020358 - 10 Feb 2023

Viewed by 1065

Abstract

The extraction of cobalt from secondary resources has become crucial, as cobalt has been identified as a strategically important and critical raw material due to the high risks of supply chain disruptions. In this work, selective sulfation roasting was investigated as a potential recycling strategy to extract cobalt and lithium from an industrial lithium cobalt oxide (LCO)-rich black mass. Additionally, the effect of graphite on metal extraction was studied. In the first set of experiments, the sieved black mass fraction containing both cathode and anode materials was directly roasted in a predetermined composition of gas mixtures of SO₂, O₂, and Ar for 1 h at 850 °C. The gas composition was determined from Kellogg’s diagram to allow for the selective sulfation of Co and Li. In another set of experiments, the carbon present in the black mass was first removed by roasting the material in Ar for 2 h and then in an Ar and O₂ gas mixture for five hours at 600 °C. Afterward, selective sulfation roasting was performed in mixtures of SO₂, O₂, and Ar gas similar to the previous set of experiments. For comparison, similar experiments were performed at 800 °C. The sulfation roasted black mass was leached in water to study the efficiency of Co extraction into the solution. Interestingly, the presence of carbon was found to be beneficial for Co extraction. The extraction efficiency for the first case (with carbon present in the raw material) was observed to be more than three times higher than in the second case (with carbon removed) for sulfation at 850 °C. The extraction efficiency and purity of the extracted Co were found to be better for higher temperature sulfation roasting conditions due to faster reaction kinetics. It was also found that almost all of the Li could be recovered while extracting Co. The maximum efficiency of the extraction was 99.51% Li and 61.21% Co for roasting under a gas flow of 10% SO₂-10% O₂-Ar at 850 °C for 60 min. These results suggest that Co and Li can be selectively extracted from the black mass by sulfation roasting pre-treatment followed by leaching in water. In holistic processing, the leach residue can then be further subjected to battery metal processing by state-of-the-art methods. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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Open AccessArticle

Optimization of a Pyrometallurgical Process to Efficiently Recover Valuable Metals from Commercially Used Lithium-Ion Battery Cathode Materials LCO, NCA, NMC622, and LFP

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Metals 2022, 12(10), 1642; https://doi.org/10.3390/met12101642 - 29 Sep 2022

Cited by 1 | Viewed by 1390

Abstract

With an ever-growing demand for critical raw materials for the production of lithium-ion batteries and a price increase of respective commodities, an ever louder call from the industry for efficient recycling technologies can be noticed. So far, state-of-the-art industry-scaled pyrometallurgical recycling technologies all suffer from the same bottleneck of lithium slagging. At the Chair of Thermal Processing Technology at Montanuniversitaet Leoben, a novel reactor was developed to recover lithium and phosphorus via the gas phase in a pyrometallurgical process. Critical elements such as Li, Ni, Co, and Mn of the commercially used cathode materials LCO (LiCoO₂), LFP (LiFePO₄), NCA (LiNi_0.8Co_0.15Al_0.05O₂), and NMC622 (LiNi_0.6Mn_0.2Co_0.2) were analyzed in a batch version of the so-called InduRed reactor concept. The analyses underline that the reactor concept is highly suitable for an efficient recovery for the metals Ni and Co and that slagging of Li can not only be largely prohibited, but the elements lithium and phosphorous can even be recovered from the gas phase. Plant engineering issues were also considered for further development toward a continuous process. The MgO crucible used shows significant diffusion of various elements from the battery material, which is why the choice of crucible material still requires in-depth research. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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Open AccessArticle

Environmentally Friendly Recovery of Lithium from Lithium–Sulfur Batteries

Lilian Schwich

and

Bernd Friedrich

Metals 2022, 12(7), 1108; https://doi.org/10.3390/met12071108 - 28 Jun 2022

Cited by 3 | Viewed by 1666

Abstract

In the context of the rising demand for electric storage systems, lithium–sulfur batteries provide an attractive solution for low-weight and high-energy battery systems. Considering circular economy for new technologies, it is necessary to assure the raw material requirements for future generations. Therefore, metallurgical recycling processes are required. Since lithium is the central and most valuable element used in lithium–sulfur batteries, this study presents an environmentally friendly and safe process for lithium recovery as lithium carbonate. The developed and experimentally performed process is a combination of thermal and hydrometallurgical methods. Firstly, the battery cells are thermally deactivated to mechanically extract black mass. Then, water leaching of the black mass in combination with using CO₂, instead of emitting it, can mobilize lithium by >90% as solid product. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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Open AccessArticle

Recovering Value from End-of-Life Batteries by Integrating Froth Flotation and Pyrometallurgical Copper-Slag Cleaning

and

Rodrigo Serna-Guerrero

Metals 2022, 12(1), 15; https://doi.org/10.3390/met12010015 - 22 Dec 2021

Cited by 2 | Viewed by 2259

Abstract

In this study, industrial lithium-ion battery (LIB) waste was treated by a froth flotation process, which allowed selective separation of electrode particles from metallic-rich fractions containing Cu and Al. In the flotation experiments, recovery rates of ~80 and 98.8% for the cathode active elements (Co, Ni, Mn) and graphite were achieved, respectively. The recovered metals from the flotation fraction were subsequently used in high-temperature Cu-slag reduction. In this manner, the possibility of using metallothermic reduction for Cu-slag reduction using Al-wires from LIB waste as the main reductant was studied. The behavior of valuable (Cu, Ni, Co, Li) and hazardous metals (Zn, As, Sb, Pb), as a function of time as well as the influence of Cu-slag-to-spent battery (SB) ratio, were investigated. The results showcase a suitable process to recover copper from spent batteries and industrial Cu-slag. Cu-concentration decreased to approximately 0.3 wt.% after 60 min reduction time in all samples where Cu/Al-rich LIB waste fraction was added. It was also showed that aluminothermic reduction is effective for removing hazardous metals from the slag. The proposed process is also capable of recovering Cu, Co, and Ni from both Cu-slag and LIB waste, resulting in a secondary Cu slag that can be used in various applications. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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Review

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Open AccessFeature PaperReview

Cobalt Recovery from Li-Ion Battery Recycling: A Critical Review

Amilton Barbosa Botelho Junior

Srecko Stopic

Bernd Friedrich

Jorge Alberto Soares Tenório

and

Denise Crocce Romano Espinosa

Metals 2021, 11(12), 1999; https://doi.org/10.3390/met11121999 - 10 Dec 2021

Cited by 19 | Viewed by 5423

Abstract

The increasing demand for Li-ion batteries for electric vehicles sheds light upon the Co supply chain. The metal is crucial to the cathode of these batteries, and the leading global producer is the D.R. Congo (70%). For this reason, it is considered critical/strategic due to the risk of interruption of supply in the short and medium term. Due to the increasing consumption for the transportation market, the batteries might be considered a secondary source of Co. The outstanding amount of spent batteries makes them to a core of urban mining warranting special attention. Greener technologies for Co recovery are necessary to achieve sustainable development. As a result of these sourcing challenges, this study is devoted to reviewing the techniques for Co recovery, such as acid leaching (inorganic and organic), separation (solvent extraction, ion exchange resins, and precipitation), and emerging technologies—ionic liquids, deep eutectic solvent, supercritical fluids, nanotechnology, and biohydrometallurgy. A dearth of research in emerging technologies for Co recovery from Li-ion batteries is discussed throughout the manuscript within a broader overview. The study is strictly connected to the Sustainability Development Goals (SDG) number 7, 8, 9, and 12. Full article

(This article belongs to the Special Issue New Science Based Concepts for Increased Efficiency in Battery Recycling 2023)

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