Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)

Recent studies in hydrometallurgy are focused on developing eco-friendly and selective leach agents such as organic acids. These agents can extract metal ions, which are usually separated through precipitation methods. When traditional methods are used, the separation is complex and time-consuming,...

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Main Authors: Dominik Schmitz, Hariaman Prasetyo, Alexander Birich, Rungsima Yeetsorn, Bernd Friedrich
Format: Article
Language:English
Published: MDPI AG 2024-01-01
Series:Metals
Subjects:
Online Access:https://www.mdpi.com/2075-4701/14/1/80
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author Dominik Schmitz
Hariaman Prasetyo
Alexander Birich
Rungsima Yeetsorn
Bernd Friedrich
author_facet Dominik Schmitz
Hariaman Prasetyo
Alexander Birich
Rungsima Yeetsorn
Bernd Friedrich
author_sort Dominik Schmitz
collection DOAJ
description Recent studies in hydrometallurgy are focused on developing eco-friendly and selective leach agents such as organic acids. These agents can extract metal ions, which are usually separated through precipitation methods. When traditional methods are used, the separation is complex and time-consuming, and each metal cation is required to be isolated separately. Moreover, extracted metal salts are subsequently recombined in the regeneration of cathode materials. To simplify this, a novel simultaneous precipitation approach has been developed, allowing the separation of metal salts that can directly contribute to regenerating novel cathode materials, bypassing the need for separate isolation. This study aimed to recover cobalt, nickel, and manganese from the organic leach solution of spent lithium-ion batteries (LIBs) through co-precipitation of metal oxalates. The investigation includes the selection of organic acids and the best parameters for the leaching process, as well as testing different molar ratios of the metals M<sup>2+</sup> (M = Co, Ni, Mn) to oxalic acid (1:3, 1:4.5, 1:6, and 1:7.5) to examine the effects of the precipitating agent on the recovery percentages of the metals. The findings indicate that 2 M citric acid and 4 vol% H<sub>2</sub>O<sub>2</sub> is the optimal parameter in the leaching process. Meanwhile, in the co-precipitation process, an increase in the molar ratio leads to a corresponding rise in the resulting metal recoveries. At the ratio of 1:7.5, cobalt, nickel, and manganese were recovered to the extent of 99.26%, 98.93%, and 94.01%, respectively. Nevertheless, at the increased molar ratio, the co-extraction of lithium and aluminum was observed, resulting in reduced selectivity and decreased precipitate purity.
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spelling doaj.art-4630fa33522944d1947ff162189ff7eb2024-01-26T17:41:20ZengMDPI AGMetals2075-47012024-01-011418010.3390/met14010080Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)Dominik Schmitz0Hariaman Prasetyo1Alexander Birich2Rungsima Yeetsorn3Bernd Friedrich4IME Process Metallurgy and Metal Recycling, RWTH Aachen University, Intzestrasse 3, 52056 Aachen, GermanyThe Sirindhorn International Thai-German Graduate School of Engineering, King Mongkut’s University of Technology North Bangkok, Bangkok 10800, ThailandIME Process Metallurgy and Metal Recycling, RWTH Aachen University, Intzestrasse 3, 52056 Aachen, GermanyThe Sirindhorn International Thai-German Graduate School of Engineering, King Mongkut’s University of Technology North Bangkok, Bangkok 10800, ThailandIME Process Metallurgy and Metal Recycling, RWTH Aachen University, Intzestrasse 3, 52056 Aachen, GermanyRecent studies in hydrometallurgy are focused on developing eco-friendly and selective leach agents such as organic acids. These agents can extract metal ions, which are usually separated through precipitation methods. When traditional methods are used, the separation is complex and time-consuming, and each metal cation is required to be isolated separately. Moreover, extracted metal salts are subsequently recombined in the regeneration of cathode materials. To simplify this, a novel simultaneous precipitation approach has been developed, allowing the separation of metal salts that can directly contribute to regenerating novel cathode materials, bypassing the need for separate isolation. This study aimed to recover cobalt, nickel, and manganese from the organic leach solution of spent lithium-ion batteries (LIBs) through co-precipitation of metal oxalates. The investigation includes the selection of organic acids and the best parameters for the leaching process, as well as testing different molar ratios of the metals M<sup>2+</sup> (M = Co, Ni, Mn) to oxalic acid (1:3, 1:4.5, 1:6, and 1:7.5) to examine the effects of the precipitating agent on the recovery percentages of the metals. The findings indicate that 2 M citric acid and 4 vol% H<sub>2</sub>O<sub>2</sub> is the optimal parameter in the leaching process. Meanwhile, in the co-precipitation process, an increase in the molar ratio leads to a corresponding rise in the resulting metal recoveries. At the ratio of 1:7.5, cobalt, nickel, and manganese were recovered to the extent of 99.26%, 98.93%, and 94.01%, respectively. Nevertheless, at the increased molar ratio, the co-extraction of lithium and aluminum was observed, resulting in reduced selectivity and decreased precipitate purity.https://www.mdpi.com/2075-4701/14/1/80battery recyclingspent lithium-ion batteriesorganic acid leachingco-precipitationoxalic acidmetal oxalate
spellingShingle Dominik Schmitz
Hariaman Prasetyo
Alexander Birich
Rungsima Yeetsorn
Bernd Friedrich
Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)
Metals
battery recycling
spent lithium-ion batteries
organic acid leaching
co-precipitation
oxalic acid
metal oxalate
title Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)
title_full Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)
title_fullStr Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)
title_full_unstemmed Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)
title_short Co-Precipitation of Metal Oxalates from Organic Leach Solution Derived from Spent Lithium-Ion Batteries (LIBs)
title_sort co precipitation of metal oxalates from organic leach solution derived from spent lithium ion batteries libs
topic battery recycling
spent lithium-ion batteries
organic acid leaching
co-precipitation
oxalic acid
metal oxalate
url https://www.mdpi.com/2075-4701/14/1/80
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