
(a) Scheme of density-based separation of oxide SSB components using heavy liquids, such as the Clerici solution or aqueous solutions of polytungstate, (b) density-based separation of thiophosphate (top) and oxide (bottom) rich fractions from an intimately ground mixture of Li3PS4, LiMn2O4 and Li4Ti5O12, (c) diffraction patterns of the low-density fraction and the high-density fraction, showing strong amorphization of the low-density fraction of LiBr.
Figures of the Article
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Schematic flow sheet, showing the different recycling approaches for conventional LIBs. After the pre-treatment step (separation of cathode materials from other components), different recycling strategies (e.g. pyro-, hydrometallurgy and direct recycling) can be used in order to recover metals for the further re-synthesis of the cathode materials.
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Suggested process flow of the developed hydrometallurgical recycling procedure of a LLZ + NMC cell system (a) complete dissolution of electrolyte and electrode materials within a single leaching step in strong acidic medium and (b) selective leaching approach for separation of the electrode from the electrolyte under moderate acidic conditions. Recovery of individual elements via a multi-step chemical precipitation process at specific pH levels. Reproduced from [13]. CC BY 4.0.
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Flow-sheet of hydrometallurgical process (a) acid leaching with subsequent alkali precipitation in HCl medium at pH = 1 within an LFP/LLZO/LTO system. Recovered materials for consecutive re-synthesis are stated in red color. Reproduced from [108]. CC BY 4.0. (b) Step-by-step approach for the recovering of individual components from an LTO/LLZTO/NMC cell system using different concentrations of citric acid as the leaching medium. [115] John Wiley & Sons. [© 2023 The Authors. ChemSusChem published by Wiley-VCH GmbH].
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(a) Scheme of density-based separation of oxide SSB components using heavy liquids, such as the Clerici solution or aqueous solutions of polytungstate, (b) density-based separation of thiophosphate (top) and oxide (bottom) rich fractions from an intimately ground mixture of Li3PS4, LiMn2O4 and Li4Ti5O12, (c) diffraction patterns of the low-density fraction and the high-density fraction, showing strong amorphization of the low-density fraction of LiBr.
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Comparison of solubility of Li3PS4 in different solvents. Solvents that can dissolve the material fully are highlighted by a red rectangle, whereas solvents that have been reported to be used for synthesis are marked with a gray rectangle. Reprinted with permission from [132]. Copyright (2023) American Chemical Society.
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Suggested process flow for industrial application. Process shows a multi-step direct recycling approach. After the cell packaging dissembling (a), SSE is being dissolved and separated from the cathode material via centrifugation (b) and (c). Solution is evaporated and SSE can be recovered with a subsequent thermal treatment. Separated cathode material can further be regenerated via re-lithiation process (d) and (e). Reproduced from [15]. CC BY 4.0.
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Schematic of a conceptual process flow for the recycling of SSBs, showing the basic principle of a hydrometallurgical (above) and direct recycling/dissolution-based separation process (below). Hydrometallurgy is illustrated as an acid leaching with a subsequent chemical precipitation process. Precursor materials are being recovered at specific pH-levels and further used for the re-synthesis of electrolyte and electrode materials (marked with a green dashed line). Direct recycling/dissolution-based separation method shows the dissolution of the electrolyte in a suitable solvent, thus its separation from the electrode materials. After filtration, the solvent can be evaporated and re-crystallized. Electrode materials can further be treated via hydrometallurgy (marked with a gray dashed line).
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Comparison of (a) a consecutive development of battery manufacturing and recycling, (b) to a product recovery-oriented design of the manufacturing process.
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