Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries

The selective separation of lithium from spent ternary positive materials is achieved through hydrogen reduction followed by water leaching. Almost 98% of the Li is transformed into soluble LiOH⋅H<sub>2</sub>O, while the Ni, Co and Mn species are all transformed into insoluble metals or...

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Main Authors: Yong Guo, Fupeng Liu, Feixiong Chen, Zaoming Chen, Hong Zeng, Tao Zhang, Changquan Shen
Format: Article
Language:English
Published: MDPI AG 2024-01-01
Series:Batteries
Subjects:
Online Access:https://www.mdpi.com/2313-0105/10/1/28
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author Yong Guo
Fupeng Liu
Feixiong Chen
Zaoming Chen
Hong Zeng
Tao Zhang
Changquan Shen
author_facet Yong Guo
Fupeng Liu
Feixiong Chen
Zaoming Chen
Hong Zeng
Tao Zhang
Changquan Shen
author_sort Yong Guo
collection DOAJ
description The selective separation of lithium from spent ternary positive materials is achieved through hydrogen reduction followed by water leaching. Almost 98% of the Li is transformed into soluble LiOH⋅H<sub>2</sub>O, while the Ni, Co and Mn species are all transformed into insoluble metals or their oxides, so the recovery of Ni, Co and Mn at this stage is challenging. The traditional acid leaching process has drawbacks such as high oxidant consumption, the low recovery of valuable metals and high production costs. Thus, sulfation roasting followed by water leaching was studied in this project. The leaching levels of Ni, Co, Mn and Al reached 87.13%, 99.87%, 96.21% and 94.95%, respectively, with 1.4 times the theoretical amount of sulfuric acid used at 180 °C for 120 min. To avoid the adverse effects of Mn and Al on the quality of the Ni and Co sulfate products, Mn<sup>2+</sup> was first separated and precipitated via the KMnO<sub>4</sub> oxidation–precipitation method, and >98% of the Mn was removed and precipitated within 30 min with a K<sub>p</sub>/K<sub>t</sub> (ratio of actual usage to theoretical usage of KMnO<sub>4</sub>) of 1.0 at pH = 2.0 and 25 °C. After removal of the Mn, the solvent extraction method was adopted by using P204 as an extractant to separate Al. More than 98% of the Al was extracted in 30 min with 20% (<i>v</i>/<i>v</i>) P204 + 10% (<i>v</i>/<i>v</i>) TBP with an A/O ratio of 1:1 at 30 °C. This optimized process for extracting lithium residues improved the hydrogen reduction process of waste lithium batteries and will enable industrialization of the developed processes.
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spelling doaj.art-e5b2f8f346294d29b6ecf7f8f702748c2024-01-26T15:05:08ZengMDPI AGBatteries2313-01052024-01-011012810.3390/batteries10010028Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium BatteriesYong Guo0Fupeng Liu1Feixiong Chen2Zaoming Chen3Hong Zeng4Tao Zhang5Changquan Shen6Yichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaYichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaYichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaYichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaYichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaYichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaYichun Lithium New Energy Industry Research Institute, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaThe selective separation of lithium from spent ternary positive materials is achieved through hydrogen reduction followed by water leaching. Almost 98% of the Li is transformed into soluble LiOH⋅H<sub>2</sub>O, while the Ni, Co and Mn species are all transformed into insoluble metals or their oxides, so the recovery of Ni, Co and Mn at this stage is challenging. The traditional acid leaching process has drawbacks such as high oxidant consumption, the low recovery of valuable metals and high production costs. Thus, sulfation roasting followed by water leaching was studied in this project. The leaching levels of Ni, Co, Mn and Al reached 87.13%, 99.87%, 96.21% and 94.95%, respectively, with 1.4 times the theoretical amount of sulfuric acid used at 180 °C for 120 min. To avoid the adverse effects of Mn and Al on the quality of the Ni and Co sulfate products, Mn<sup>2+</sup> was first separated and precipitated via the KMnO<sub>4</sub> oxidation–precipitation method, and >98% of the Mn was removed and precipitated within 30 min with a K<sub>p</sub>/K<sub>t</sub> (ratio of actual usage to theoretical usage of KMnO<sub>4</sub>) of 1.0 at pH = 2.0 and 25 °C. After removal of the Mn, the solvent extraction method was adopted by using P204 as an extractant to separate Al. More than 98% of the Al was extracted in 30 min with 20% (<i>v</i>/<i>v</i>) P204 + 10% (<i>v</i>/<i>v</i>) TBP with an A/O ratio of 1:1 at 30 °C. This optimized process for extracting lithium residues improved the hydrogen reduction process of waste lithium batteries and will enable industrialization of the developed processes.https://www.mdpi.com/2313-0105/10/1/28spent lithium batterieshydrogen reductionsulfation roastinglithiumaluminum removal
spellingShingle Yong Guo
Fupeng Liu
Feixiong Chen
Zaoming Chen
Hong Zeng
Tao Zhang
Changquan Shen
Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries
Batteries
spent lithium batteries
hydrogen reduction
sulfation roasting
lithium
aluminum removal
title Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries
title_full Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries
title_fullStr Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries
title_full_unstemmed Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries
title_short Recycling of Valuable Metals from the Priority Lithium Extraction Residue Obtained through Hydrogen Reduction of Spent Lithium Batteries
title_sort recycling of valuable metals from the priority lithium extraction residue obtained through hydrogen reduction of spent lithium batteries
topic spent lithium batteries
hydrogen reduction
sulfation roasting
lithium
aluminum removal
url https://www.mdpi.com/2313-0105/10/1/28
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