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Membranes 2022, 12, 373 19 of 29 500–600 ◦C, however, vacuum was applied to avoid high-temperature aluminium brittle- ness [132]. Although the thermal treatment method has proven to be highly productive in terms of operational efficiency and high throughput, it has a disadvantage of producing hazardous gases due to high-temperature decomposition reactions. To avoid high energy consumption, facile mechanical separation methods including crushing, grinding, sieving and magnetic separation have been reported [133]. Shin et al. concluded that the separation efficiency of targeted metals can be enhanced by integrating mechanical methods before the metal-leaching process [134]. Both mechanical and thermal treatment methods have the advantages of being straight- forward and convenient, however, suffer from producing hazardous chemicals (Table 1) [135]. Even though most pre-treatment processes have successfully been applied in different industries across the world, there are still great developments to be researched to improve the process. Such research should include methods that are not only economically feasible, but simultaneously reduce the environmental footprints. 4.1.2. Metal Extraction Process Metal extraction is the most significant part of the LIBs recycling process. In the recent decade, hydro-metallurgy, pyro-metallurgy, bio-metallurgy, and hybrid processes are widely used in industries not only for the recycling and refining of lithium but also for the extraction of other metals including nickel, copper, cobalt, and aluminium. In this section, the above-mentioned metal-extraction techniques are reviewed in terms of their strengths and weaknesses within current recycling processes. Pyro-Metallurgy Processes Pyro-metallurgical processes work on the principle of high-temperature smelting, typically in the presence of a reducing agent (e.g., coke) [135]. Normally, these processes do not require pre-treatment and the spent LIBs are directly added to the smelting furnace where they are heated beyond their melting point. Consequently, reducing the amount of carbon by converting it into alloys. The majority of the energy for the burning is provided by the combustion of the carbonaceous compounds, plastics and other volatile matter already present inside the spent LIBs. This high-temperature reductive alloy formation is followed by a secondary recovery stage through leaching. This is typically achieved with various reagents such as water or various acids (e.g., sulphuric acid (H2SO4)) [136]. Finally, solvent extraction is employed to obtain the products containing Ni, Fe, Co, and Mn. The drawback of this recovery process is the loss of lithium due to slag formation [109]. Georgi- Maschler et al. improved lithium recovery from slag by applying secondary leaching using sulphuric acid (H2SO4) [40]. In another study, Hu et al. proposed a series of steps for enhanced lithium recovery from LIBs. The method starts with the roasting of LIBs under an argon environment followed by a water leaching process to extract Li2CO3 alongside other metal components. The mixture is then subjected to CO2 to convert Li2CO3 to LiHCO3. Finally, the lithium is recovered through evaporation crystallization [137]. Träger et al. studied lithium recovery through evaporation at a temperature beyond 1400 ◦C, however it proved to be economically inviable due to high demand for energy consumption [138]. Although lithium recovery from LIBs using pyro-metallurgical processes is simple, they have obvious disadvantages such as high operational cost, lithium losses and risk of secondary pollution [45]. To mitigate the operational hazards, current research has been focused on either process refinement or hybrid methodologies, e.g., pyro-metallurgy coupled with hydro-metallurgy [2]. Hydro-Metallurgy Processes Similar to pyro-metallurgy, hydro-metallurgical processes typically initiate with LIB pre-treatment followed by leaching, precipitation and solvent extraction. The effectiveness of a leaching process mainly depends upon the process parameters, including the type and concentration of the leaching reagent, process temperature, time duration, solid/liquidPDF Image | Lithium Harvesting using Membranes
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