Summary of Pretreatment of Waste Lithium-Ion Batteries and Recycling of Valuable Metal Materials: A Review
Abstract
:1. Introduction
2. Pre-Processing Technology
2.1. Discharge
2.2. Crushing, Screening, and Sorting
3. The Technology of the Material-Recycling Steps
3.1. Combination of Pyrometallurgical Technology and Hydrometallurgical Technology
3.2. The Inorganic Acid Hydrometallurgy Technology
3.3. The Organic Acid Leaching Method
3.4. The Direct Recycling Technology
3.5. The Biometallurgy Method
3.6. Summary of Technologies for the Material-Recycling Phase
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
Abbreviations
SEM | Scanning electron microscopy |
XRD | X-ray Diffraction |
References
- Zhou, Z. Strong growth in global electric vehicle sales. People’s Daily, 1 March 2023. [Google Scholar] [CrossRef]
- BorgWarner. BorgWarner Reports First Quarter 2023 Results, Expects 2023 eProduct Sales of $2.3 Billion to $2.6 Billion. BorgWarner Reports, 4 May 2023.
- Dehghani-Sanij, A.; Tharumalingam, E.; Dusseault, M. Study of energy storage systems and environmental challenges of batteries. Renew. Sustain. Energy Rev. 2019, 104, 192–208. [Google Scholar] [CrossRef]
- Wei, X.; Zhang, M.; Miao, B.; Liu, R. Volumetric capacity enhancement in LiFePO4 cathodes by hot isostatic pressing. Scr. Mater. 2021, 194, 113638. [Google Scholar] [CrossRef]
- Su, Y. Comparative Analysis of Lithium Iron Phosphate Battery and Ternary Lithium Battery. In Proceedings of the 2021 International Conference on Materials Chemistry and Environmental Engineering (CONF-MCEE 2021), Online, 11–16 November 2021; pp. 425–431. [Google Scholar] [CrossRef]
- Saeed, A.M.N.; Hezam, A.; Al-Gunaid, M.Q.A.; Somesh, T.E.; Siddaramaiah. Effect of ethylene carbonate on properties of PVP-CsAlO;-LiClO;solid polymer electrolytes. Polym. Technol. Mater. 2021, 60, 132–146. [Google Scholar] [CrossRef]
- Liang, Y.; Zhao, C.Z.; Yuan, H.; Chen, Y.; Zhang, W.; Huang, J.Q.; Yu, D.; Liu, Y.; Titirici, M.M.; Chueh, Y.L.; et al. A review of rechargeable batteries for portable electronic devices. InfoMat 2019, 1, 6–32. [Google Scholar] [CrossRef]
- Stich, M.; Göttlinger, M.; Kurniawan, M. Hydrolysis of LiPF6 in Carbonate-Based Electrolytes for Lithium-Ion Batteries and Aqueous Media. J. Phys. Chem. 2018, 122, 8836–8842. [Google Scholar] [CrossRef]
- Li, J.; Wang, G.; Xu, Z. Generation and detection of metal ions and volatile organic compounds (VOCs) emissions from the pretreatment processes for recycling spent lithium-ion batteries. Waste Manag. 2016, 52, 221–227. [Google Scholar] [CrossRef]
- Brückner, L.; Frank, J.; Elwert, T. Industrial Recycling of Lithium-Ion Batteries—A Critical Review of Metallurgical Process Routes. Metals 2020, 10, 1107. [Google Scholar] [CrossRef]
- Ma, X.; Ge, P.; Wang, L.; Sun, W.; Bu, Y.; Sun, M.; Yang, Y. The Recycling of Spent Lithium-Ion Batteries: Crucial Flotation for the Separation of Cathode and Anode Materials. Molecules 2023, 28, 4081. [Google Scholar] [CrossRef] [PubMed]
- Fahimi, A.; Alessandri, I.; Cornelio, A.; Frontera, P.; Malara, A.; Mousa, E.; Ye, G.; Valentim, B.; Bontempi, E. A microwave-enhanced method able to substitute traditional pyrometallurgy for the future of metals supply from spent lithium-ion batteries. Resour. Conserv. Recycl. 2023, 194, 106989. [Google Scholar] [CrossRef]
- An, B.; Lee, T.; Khan, T.T.; Seo, H.; Hwang, H.J.; Jun, Y. Optical and quantitative detection of cobalt ion using graphitic carbon nitride-based chemosensor for hydrometallurgy of waste lithium-ion batteries. Chemosphere 2023, 315, 137789. [Google Scholar] [CrossRef]
- Kanesalingam, B.; Fernando, W.A.M.; Panda, S.; Jayawardena, C.; Attygalle, D.; Amarasinghe, D.A.S. Harnessing the Capabilities of Microorganisms for the Valorisation of Coal Fly Ash Waste through Biometallurgy. Minerals 2023, 13, 724. [Google Scholar] [CrossRef]
- Yu, D. Pretreatment options for the recycling of spent lithium-ion batteries: A comprehensive review. Miner. Eng. 2021, 173, 107–218. [Google Scholar] [CrossRef]
- Gao, T.; Dai, T.; Fan, N.; Han, Z.; Gao, X. Comprehensive review and comparison on pretreatment of spent lithium-ion battery. J. Environ. Manag. 2024, 363, 121314. [Google Scholar] [CrossRef] [PubMed]
- Seoa, K.; Jaeyeon, B. A comprehensive review on the pretreatment process in lithium-ion battery recycling. J. Clean. Prod. 2021, 294, 126329. [Google Scholar] [CrossRef]
- Jiang, L.; Zheng, W.; Zhang, G. Research on green discharge technology for pretreatment of waste lithium-ion batteries. J. Cent. South Univ. 2023, 54, 684–693. [Google Scholar] [CrossRef]
- Yao, L.P.; Zeng, Q.; Qi, T.; Li, J. An environmentally friendly discharge technology to pretreat spent lithium-ion batteries. J. Clean. Prod. 2020, 245, 118820. [Google Scholar] [CrossRef]
- Granata, G.; Pagnanelli, F.; Moscardini, E.; Takacova, Z.; Havlik, T.; Toro, L. Simultaneous recycling of nickel metal hydride, lithium ion and primary lithium batteries: Accomplishment of European Guidelines by optimizing mechanical pre-treatment and solvent extraction operations. J. Power Sources 2012, 212, 205–211. [Google Scholar] [CrossRef]
- Zhang, T.; He, Y.; Ge, L.; Fu, R.; Zhang, X.; Huang, Y. Characteristics of wet and dry crushing methods in the recycling process of spent lithium-ion batteries. J. Power Sources 2013, 240, 766–771. [Google Scholar] [CrossRef]
- Nan, J.; Han, D.; Yang, M.; Cui, M.; Hou, X. Recovery of metal values from a mixture of spent lithium-ion batteries and nickel-metal hydride batteries. Hydrometallurgy 2006, 84, 75–80. [Google Scholar] [CrossRef]
- Meshram, P.; Somani, H.; Pandey, B.D.; Mankhand, T.R.; Deveci, H.; Abhilash. Two stage leaching process for selective metal extraction from spent nickel metal hydride batteries. J. Clean. Prod. 2017, 157, 322–332. [Google Scholar] [CrossRef]
- Shin, S.M.; Kim, N.H.; Sohn, J.S.; Yang, D.H.; Kim, Y.H. Development of a metal recovery process from Li-ion battery wastes. Hydrometallurgy 2005, 79, 172–181. [Google Scholar] [CrossRef]
- Li, J.; Wang, G.; Xu, Z. Environmentally-friendly oxygen-free roasting/wet magnetic separation technology for in situ recycling cobalt, lithium carbonate and graphite from spent LiCoO2/graphite lithium batteries. J. Hazard. Mater. 2016, 302, 97–104. [Google Scholar] [CrossRef] [PubMed]
- Yu, J.; He, Y.; Li, H.; **. Carbon Energy 2022, 9, 104789. [Google Scholar] [CrossRef]
- Shi, Y.; Chen, G.; Chen, Z. Effective regeneration of LiCoO2 from spent lithium-ion batteries: A direct approach towards high-performance active particles. Green Chem. 2018, 20, 851–862. [Google Scholar] [CrossRef]
- Yang, J.; Wang, W.; Yang, H.; Wang, D. One-pot compositional and structural regeneration of degraded LiCoO2 for directly reusing it as a high-performance lithium-ion battery cathode. Green Chem. 2020, 22, 6489–6496. [Google Scholar] [CrossRef]
- Li, J.; Zhong, S.; **ong, D.; Chen, H. Synthesis and electrochemical performances of LiCoO2 recycled from the incisors bound of Li-ion batteries. Rare Met. 2009, 28, 328–332. [Google Scholar] [CrossRef]
- Li, L.; Chen, R.; Sun, F.; Wu, F.; Liu, J. Preparation of LiCoO2 films from spent lithium-ion batteries by a combined recycling process. Hydrometallurgy 2011, 108, 220–225. [Google Scholar] [CrossRef]
- Zhou, S.; Zhang, Y.; Meng, Q.; Dong, P.; Yang, X.; Liu, P.; Li, Q.; Fei, Z. Recycling of spent LiCoO2 materials by electrolytic leaching of cathode electrode plate. J. Environ. Chem. Eng. 2021, 9, 104789. [Google Scholar] [CrossRef]
- Jegan, J.R. A review on the recycling of spent lithium-ion batteries (LIBs) by the bioleaching approach. Chemosphere 2021, 282, 130944. [Google Scholar] [CrossRef]
- Yu, Z. Recent advances in the recovery of metals from waste through biological processes. Bioresour. Technol. 2020, 297, 122416. [Google Scholar] [CrossRef] [PubMed]
- Gumulya, Y.; Boxall, N.J.; Khaleque, H.N.; Santala, V.; Carlson, R.P.; Kaksonen, A.H. In a quest for engineering acidophiles for biomining applications: Challenges and opportunities. Genes 2018, 9, 116. [Google Scholar] [CrossRef]
- Jegan Roy, J.; Srinivasan, M.; Cao, B. Bioleaching as an Eco-Friendly Approach for Metal Recovery from Spent NMC-Based Lithium-Ion Batteries at a High Pulp Density. ACS Sustain. Chem. Eng. 2021, 197, 3060–3069. [Google Scholar] [CrossRef]
- Ghassa, S.; Farzanegan, A.; Gharabaghi, M.; Abdollahi, H. Novel bioleaching of waste lithium ion batteries by mixed moderate thermophilic microorganisms, using iron scrap as energy source and reducing agent. Hydrometallurgy 2020, 197, 105465. [Google Scholar] [CrossRef]
- Bahaloo-Horeh, N.; Mousavi, S.M. Enhanced recovery of valuable metals from spent lithium-ion batteries through optimization of organic acids produced by Aspergillus niger. Waste Manag. 2017, 60, 666–679. [Google Scholar] [CrossRef] [PubMed]
- Bahaloo-Horeh, N.; Mousavi, S.M.; Baniasadi, M. Use of adapted metal tolerant Aspergillus niger to enhance bioleaching efficiency of valuable metals from spent lithium-ion mobile phone batteries. J. Clean. Prod. 2018, 197, 1546–1557. [Google Scholar] [CrossRef]
- Chen, G.; Shi, H. Multi-scale analysis of nickel ion tolerance mechanism for thermophilic Sulfobacillus thermosulfidooxidans in bioleaching. J. Hazard. Mater. 2022, 443, 130245. [Google Scholar] [CrossRef]
- Zhuang, W.-Q.; Fitts, J.P.; Ajo-Franklin, C.M.; Maes, S.; Alvarez-Cohen, L.; Hennebel, T. Recovery of critical metals using biometallurgy. Curr. Opin. Biotechnol. 2015, 33, 327–335. [Google Scholar] [CrossRef]
- Choi, J.; Kim, J.; Kim, S.; Yun, Y. Simple, green organic acid-based hydrometallurgy for waste-to-energy storage devices: Recovery of NiMnCoC2O4 as an electrode material for pseudocapacitor from spent LiNiMnCoO2 batteries. J. Hazard. Mater. 2022, 424, 127481. [Google Scholar] [CrossRef] [PubMed]
- **a, T.; Wu, Z.; Liang, Y.; Wang, W.; Li, Y.; Tian, X.; Feng, L.; Sui, Z.; Chen, Q. Sulfonic acid functionalized covalent organic frameworks for lithium-sulfur battery separator and oxygen evolution electrocatalyst. J. Colloid Interface Sci. 2023, 645, 146–153. [Google Scholar] [CrossRef] [PubMed]
- Wang, Y.; An, N.; Wen, L. Recent progress on the recycling technology of Li-ion batteries. J. Energy Chem. 2021, 55, 391–419. [Google Scholar] [CrossRef]
- Li, J.; Luo, M.; Wang, K.; Li, G.; Zhang, G. Review of carbon dioxide mineralization of magnesium-containing materials. Carbon Neutralization 2023, 2, 574–584. [Google Scholar] [CrossRef]
- Biotech Week. Technology Recent Research from Ghent University Highlight Findings in Biotechnology (Recovery of critical metals using biometallurgy). ProQuest, 29 July 2015.
- Yang, Y.; Emenike, G. On the sustainability of lithium ion battery industry—A review and perspective. Energy Storage Mater. 2021, 36, 186–212. [Google Scholar] [CrossRef]
- Huang, B.; Pan, Z.; Su, X. Recycling of lithium-ion batteries: Recent advances and perspectives. J. Power Sources 2018, 399, 274–286. [Google Scholar] [CrossRef]
- Lv, W.; Wang, Z. A Critical Review and Analysis on the Recycling of Spent Lithium-Ion Batteries. ACS Sustain. Chem. Eng. 2018, 6, 1504–1521. [Google Scholar] [CrossRef]
(In Millions) | Q1 2022 Net Sales | FX | Q1 2023 Acquisition Impact | Organic Net Sales Change | Q1 2022 Net Sales | Organic Net Sales Change % |
---|---|---|---|---|---|---|
Air Management | USD 1768 | USD (81) | USD 2 | USD 290 | USD 1979 | 16.4% |
Drivetrain & Battery Systems | 895 | (32) | — | 92 | 955 | 10.3% |
Fuel Systems | 591 | (24) | — | 1 | 568 | 0.2 |
ePropulsion | 440 | (19) | 20 | 46 | 487 | 10.5% |
Aftermarket | 307 | (6) | — | 29 | 330 | 9.4% |
Inter-segment eliminations | (127) | — | — | (12) | (139) | — |
Net sales | USD 3874 | USD (162) | USD 22 | USD 446 | USD 4180 | 11.5% |
Solution System | Li | Ni | Co | Mn | Cu | Fe | Al | P |
---|---|---|---|---|---|---|---|---|
NaCl | 15.200 | 0.500 | 15.200 | 0.030 | 0.010 | 4.900 | 93.000 | 116.000 |
Na2SO4 | 3.400 | 0.500 | 0.490 | 0.020 | 0.010 | 1.200 | 161.000 | 12.300 |
Na2S | 0.200 | 0.300 | 0.011 | 0.020 | 0.001 | 0.200 | 4.500 | 0.030 |
Na2CO3 | 0.400 | 0.200 | 0.008 | 0.010 | 0.010 | 0.400 | 2.000 | 0.020 |
Solution System | Li | Ni | Co | Mn | Cu | Fe | Al | P | S |
---|---|---|---|---|---|---|---|---|---|
NaCl | 0.033 | 0.420 | 0.044 | 0.072 | 0.065 | 36.600 | 19.400 | 0.032 | 0.021 |
Na2SO4 | 0.014 | 0.470 | 0.016 | 0.038 | 0.036 | 44.700 | 10.800 | 0.210 | 1.670 |
Na2S | 0.007 | 0.003 | 0.005 | 0.008 | 0.004 | 26.500 | 0.180 | 0.008 | 61.400 |
Elements | Cu | Al | Li | Ni | Co | Mn |
---|---|---|---|---|---|---|
Content | 10.72 | 6.15 | 2.92 | 16.08 | 5.81 | 4.95 |
Reagent | Type of Material | Conditions | Efficiency | References |
---|---|---|---|---|
H2SO4 with H2O2 | Spent LiBs | 2.00 M H2SO4, 4.0% H2O2, 50 °C, 120 min, S/L 50 g·L−1 | >98% Co and Li were recovered | [43] |
HNO3 with H2O2 | Spent LiBs | 1.00 M HNO3, 1.7% H2O2, 75 °C, 60 min, S/L 20 g·L−1 | >95% Co and Li were recovered | [43] |
HCl | Spent LiBs | 1.75 M HCl, 50 °C, 120 min, S/L 20 g·L−1 | 90% Co and 99% Mn were recovered | [45] |
H2SO4 and H2O2; Cyanex272 | The cathode material of lithium cobalt oxide battery | 6% H2SO4, 1% H2O2, S/L 30 g·L | 80% Co and 95% Li were recovered | [46] |
Reagent | Type of Material | Conditions | Efficiency | References |
---|---|---|---|---|
Malic acid | Cathode waste materials | 1.5 M malic acid, 8 V, 300 r/min, 60 °C, 30 min | 100% Li, 99.87% Co, 99.58% Ni and 99.82% Mn were recovered | [52] |
Acetic acid, Ascorbic acid | Spent LiBs | 1.00 M acetic acid, 0.10 M ascorbic acid, 4 V, 25 °C, 70 min | 99.8% Ni, 99.8% Co, 99.8% Mn, 99.9% Li were recovered | [55] |
EDTA | Spent LiBs | 0.50 M EDTA, 353 K, 120 min, S/L 30 mL/g | 99% metal were recovered | [56] |
Gluconic acid | Spent LiBs | 1.2 M gluconic acid, H2O2 1.6 vol%, S/L 25 g/L, 75 °C, 192 min | Over 98% Li, Co, Mn, over 80% Ni were recovered | [59] |
Ascorbic acid or Employing hexuronic acid | Spent LiBs | 0.8 M acids, 70 °C, 60 min, S/L 50 g/L | 100% Li, 99.5% Cowere recovered | [60] |
DL-lactic acid | Spent LiBs | 1.00 M DL-lactic acid, 6% H2O2, 60 °C, S/L 10 g/L, 60 min | 99.8% Li, 99% Co, were recovered | [61] |
Method Type | Type of Material | Conditions | Efficiency | References |
---|---|---|---|---|
Solid-state methode | LCO | Solid-state process with direct mixing | 152.4 mA h g−1 at 0.2 C and the capacity decay rate per cycle was only 0.0313 mA h g−1 | [69] |
LCO | Solid-state process with a mixture of S-LCO, Li2CO3 and Co3O4 | 135.7 mA h g−1 at 0.5 C after 250 cycles, superior capacity retention | [65] | |
Hydrothermal method | LCO | Hydrothermal treatments with short annealing and adopted a Ni and Mn co-doped strategy | 160.23 mA h g−1 at 1 C and capacity retention of 91.2% after 100 cycles | [70] |
LCO | Hydrothermal treatment 220 °C for 4 h with short annealing (800 °C for 4 h) | 48.2 mAh g−1 (150 mA g−1, 3.0–4.3 V), 91.2% after 100 cycles | [71] | |
Eutectic medium method | LOC | Eutectic salts LiOH-KOH-Li2CO3 | 144 mA h g−1, an excellent cycling stability of 92.5% capacity retention after 200 cycles at 0.2 C | [72] |
LOC | Eutectic salts Li2CO3, LiOH·H2O and LiAc·2H2O | 160 mAh·g−1 between 3.0–4.3 V. The discharge capacity after cycling for 50 times is still 145.2 mAh·g−1 | [73] | |
Electrochemical method | LOC | Electrodeposition | Delivering a specific capacity of an initial discharge capacity of 127.2 mA h g−1 at 0.1 C | [74] |
LOC | Electrodeposition | The discharge capacity is 160.1 mA h g−1 in the initial cycle and 146.2 mA h g−1 in the 100th cycle, and the reversible specific capacity is up to 144.2 mA h g−1 at 5 C. | [75] |
Microorganism | Type of Material | Conditions | Efficiency | References |
---|---|---|---|---|
A. ferrooxidans | A mixture of LiCoO2-based spent LiBs | pH 2; 10% (v/v) Modified 9 K medium at pulp density 100 g/L 30 °C and 160 rpm in 72 h | Co (94%) and Li (60%) were recovered | [76] |
Consortium of moderately thermophilic bacteria | Waste LiB cells | pH 1.8; 10% inoculation at 45 °C and 130 rpm | Co recoveries reached 99.9%, Ni recoveries reached 99.7%, and Li recoveries reached 84% | [80] |
Aspergillus niger | Spent LiBs | At 26.478 (g L−1) sucrose concentration, 3.45% (V V−1) inoculum amount, pH 5.44 | 100% Cu, 100% Li, 77% Mn, and 75% Al occurred at 2% (w v−1) pulp density; 64% Co and 54% Ni recovery occurred at 1% (w v−1) | [81] |
Aspergillus niger | Spent LiBs | At a pulp density of 1% (w/v), the adapted Aspergillus niger leached | 100% Li, 94% Cu, 72% Mn, 62% Al, 45% Ni, and 38% Co were recovered | [82] |
Technology | The Level of Technical Difficulty | Economies of Scale Costs | Degree of Industrialization | Environmentally Friendly | Major Contaminants | Technological Development Points |
---|---|---|---|---|---|---|
Pyrometallurgy | Low | Low | High | Low | Sewage, exhaust gas, metal waste residue | Use low-energy devices in combination with other methods. |
Pyrometallurgy–hydrometallurgy | Medium | Medium | Medium | Medium | Sewage, exhaust gas, metal waste residue, organic solvents | The use of organic waste synergistic pyrometallurgy to achieve waste utilization, cleaner solvents |
Hydrometallurgy | Medium | Low | High | Medium | Sewage, organic solvents, exhaust gases | A cleaner extraction system with a better recycling process design |
Direct recycling | High | High | Low | High | Sewage, exhaust gases | Embark on an industrial |
Biometallurgy | High | High | Low | High | Sewage, waste microorganisms | Microorganisms that are more suitable for working in extreme environments, industrial exploration |
Disclaimer/Publisher’s Note: The statements, opinions and data contained in all publications are solely those of the individual author(s) and contributor(s) and not of MDPI and/or the editor(s). MDPI and/or the editor(s) disclaim responsibility for any injury to people or property resulting from any ideas, methods, instructions or products referred to in the content. |
© 2024 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
Share and Cite
Li, L.; Li, Y.; Zhang, G. Summary of Pretreatment of Waste Lithium-Ion Batteries and Recycling of Valuable Metal Materials: A Review. Separations 2024, 11, 196. https://doi.org/10.3390/separations11070196
Li L, Li Y, Zhang G. Summary of Pretreatment of Waste Lithium-Ion Batteries and Recycling of Valuable Metal Materials: A Review. Separations. 2024; 11(7):196. https://doi.org/10.3390/separations11070196
Chicago/Turabian StyleLi, Linye, Yuzhang Li, and Guoquan Zhang. 2024. "Summary of Pretreatment of Waste Lithium-Ion Batteries and Recycling of Valuable Metal Materials: A Review" Separations 11, no. 7: 196. https://doi.org/10.3390/separations11070196