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Toward Sustainable Li-Ion Battery Recycling: Green Metal-Organic Framework as a Molecular Sieve for the Selective Separation of Cobalt and Nickel
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0003-2112-9308
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Number of Authors: 102021 (English)In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 9, no 29, p. 9770-9778Article in journal (Refereed) Published
Abstract [en]

The growing demand for Li-ion batteries (LIBs) has made their postconsumer recycling an imperative need toward the recovery of valuable metals, such as cobalt and nickel. Nevertheless, their recovery and separation from active cathode materials in LIBs, via an efficient and environmentally friendly process, have remained a challenge. In this work, we approach a simple and green method for the selective separation of nickel ions from mixed cobalt-nickel aqueous solutions under mild conditions. We discovered that the bioinspired microporous metal-organic framework (MOF) SU-101 is a selective sorbent toward Ni2+ ions at pH 5-7 but does not adsorb Co2+ ions. According to the Freundlich isotherm, the adsorption capacity toward Ni2+ reached 100.9 mg.g(-1), while a near-zero adsorption capacity was found for Co2+ ions. Ni2+ removal from aqueous solutions was performed under mild conditions (22 degrees C and pH 5), with a high yield up to 96%. The presence of Ni2+ ions adsorbed on the surface of the material has been proven by solid-state H-1 nuclear magnetic resonance spectroscopy. Finally, the separation of Ni2+ from Co2+ from binary solutions was obtained with approximately 30% yield for Ni2+, with a near-zero adsorption of Co2+, which has been demonstrated by UV-vis spectroscopy. The ion adsorption process of Ni2+ and Co2+ ions was additionally studied by means of classical molecular dynamics calculations (force fields), which showed that the Ni2+ ions were more prone to enter the MOF canals by replacing some of their coordinated water molecules. These results offer a green pathway toward the recycling and separation of valuable metals from cobalt-containing LIBs while providing a sustainable route for waste valorization in a circular economy.

Place, publisher, year, edition, pages
2021. Vol. 9, no 29, p. 9770-9778
Keywords [en]
adsorption, metal-organic framework, battery recycling, nickel recovery, cobalt recovery
National Category
Chemical Sciences Chemical Engineering
Identifiers
URN: urn:nbn:se:su:diva-197069DOI: 10.1021/acssuschemeng.1c02146ISI: 000678435600022OAI: oai:DiVA.org:su-197069DiVA, id: diva2:1597297
Available from: 2021-09-24 Created: 2021-09-24 Last updated: 2022-11-01Bibliographically approved
In thesis
1. Sustainable recycling of Li-ion batteries
Open this publication in new window or tab >>Sustainable recycling of Li-ion batteries
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Lithium-ion batteries (LIBs) play a key role in today’s energy storage sector, finding applications in everyday use electronic devices, like smartphones, laptops or electric vehicles. Despite very good properties, such as high electric capacity and high number of charge-discharge cycles, eventually each battery in the world will be disposed and stored in a landfill, waiting for the opportunity to be recycled. Until then, spent LIBs are a serious hazard to the natural environment because of their toxic constituents, like organic electrolytes or transition metal based electrodes, and unfortunately, the majority of those used batteries will never be recycled due to a lack of profitable and sustainable methods for the recovery of battery components.

The demand for the production of new batteries is caused by the increase in the number of electronic devices being sold to end customers every year, and battery waste is an important and promising source of valuable metals, so far essential for manufacturing new electrode materials. However, the existing industrial methods for the recovery of metals from batteries, despite high yields and purity of obtained products, usually are associated with high energy demand, implementation or in situ generation of toxic chemicals, and generation of additional, non-recyclable fractions – therefore they can not be considered as sustainable.

This thesis summarizes the approaches taken during Author’s doctoral studies towards green LIBs recycling, implementing various techniques, like adsorption and electrochemistry, as well as the valorisation of spent LIBs towards environmental applications. The first and second works implement adsorption for the recovery of metal ions present in the battery cathode materials from aqueous solutions. The third work implements the production of a cobalt catalysts made from scrap LIBs cathode materials with further testing towards hydrogen evolution reaction from sodium borohydride. The fourth work implements hydrometallurgical treatment of spent LIBs cathode materials via leaching and electrochemical separation of metals. The aim is to show the possibilities for the recovery and reuse of spent battery cathode materials, as well as the environmental importance of recycling.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2022. p. 71
Keywords
batteries, recycling, metal recovery, adsorption, electrochemistry
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-210922 (URN)978-91-8014-094-2 (ISBN)978-91-8014-095-9 (ISBN)
Public defence
2022-12-16, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, and online via Zoom, public link is available at the department website, Stockholm, 13:00 (English)
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Available from: 2022-11-23 Created: 2022-11-01 Last updated: 2022-11-15Bibliographically approved

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Piątek, JędrzejBudnyak, Tetyana M.Gueret, RobinSvensson Grape, ErikJaworski, AleksanderInge, A. KenM. Rodrigues, Bruno V.Slabon, Adam

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Piątek, JędrzejBudnyak, Tetyana M.Gueret, RobinSvensson Grape, ErikJaworski, AleksanderInge, A. KenM. Rodrigues, Bruno V.Slabon, Adam
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