Research for the recycling of lithium-ion batteries (LIBs) started about 15 years ago. In recent years, several processes have been realized in small-scale industrial plants in Europe, which can be classified into two major process routes. The first one combines pyrometallurgy with subsequent hydrometallurgy, while the second one combines mechanical processing, often after thermal pre-treatment, with metallurgical processing. Both process routes have a series of advantages and disadvantages with respect to legislative and health, safety and environmental requirements, possible recovery rates of the components, process robustness, and economic factors. This review critically discusses the current status of development, focusing on the metallurgical processing of LIB modules and cells. Although the main metallurgical process routes are defined, some issues remain unsolved. Most process routes achieve high yields for the valuable metals cobalt, copper, and nickel. In comparison, lithium is only recovered in few processes and with a lower yield, albeit a high economic value. The recovery of the low value components graphite, manganese, and electrolyte solvents is technically feasible but economically challenging. The handling of organic and halogenic components causes technical difficulties and high costs in all process routes. Therefore, further improvements need to be achieved to close the LIB loop before high amounts of LIB scrap return.
Rare earth-bearing gypsum tailings from the fertilizer industry are a potential source for an economically viable and sustainable production of rare earth elements. Large quantities are generated inter alia in Catalão, Brazil, as a by-product in a fertilizer production plant. Hitherto, the gypsum has been used as soil conditioner in agriculture or was dumped. The cooperative project, “Catalão Monazite: Economical exploitation of rare earth elements from monazite-bearing secondary raw materials,” intends to extract rare earth elements from these gypsum tailings. In this paper, a chemical process route to obtain a mixed rare earth carbonate from a monazite concentrate, was investigated. The results of the digestion, leaching, and precipitation experiments are presented and discussed herein. This includes reagent choice, process parameter optimization through experimental design, mineralogical characterization of the feed material and residues, purification of the leach solution, and precipitation of the rare earth as carbonates. The results showed that a rare earth extraction of about 90% without the mobilization of key impurities is possible during a sulfuric acid digestion with two heating stages and subsequent leaching with water. In the following purification step, the remaining impurities were precipitated with ammonium solution and the rare earth elements were successfully recovered as carbonates with a mixture of ammonium solution and ammonium bicarbonate.
The processing of manganese nodules for the production of raw materials has been a subject of research for many decades. The nodules contain many valuable metals like copper, cobalt and nickel. In recent years, the German Federal Institute for Geoscience and Natural Resources developed a process for the processing of manganese nodules based on a combined pyro‐ and a hydrometallurgical route. Clausthal University of Technology was assigned to develop the hydrometallurgical process for the treatment of a FeNiCuCo alloy. The developed process consists of pressurized sulfuric acid leaching with the suppression of hydrogen gas formation, precipitation and solvent extraction.
Since several years, the lithium market is characterized by high growth rates especially due to the increasing demand for lithium-ion batteries. Therefore, the primary production is currently expanded and there is a growing interest in recycling. However, because of the chemical properties of lithium, many production processes lack efficient processes for the separation, concentration and purification of lithium. This article reviews the current use of liquid-liquid extraction (LLE) and chromatography in lithium production as well as research. Currently, the industrial application of LLE and chromatography in lithium purification is limited to the extraction of impurities and co-products. Extraction of lithium is only used as concentration step in few processes before lithium precipitation. In research and development, a wide variety of extractants and resins is investigated. In LLE, chelating extractants like crown ethers and calixarene and synergistic systems show the greatest potential. In the chromatographic separation the main focus of research lies upon cation exchange media, especially media with sulfonated ligands. However, most research is still in early development. Therefore, extensive research is needed to enable the industrial use of optimized LLE and chromatography processes in lithium production. Content TOC \o "1-3" \h \z \u HYPERLINK \l "_Toc515547308" Abstract PAGEREF _Toc515547308 \h 2 HYPERLINK \l "_Toc515547309" Content PAGEREF _Toc515547309 \h 3