An exponential market growth of Li-ion batteries (LIBs) has been observed in the past 20 years; approximately 670,000 tons of LIBs have been sold in 2017 alone. This trend will continue owing to the growing interest of consumers for electric vehicles, recent engagement of car manufacturers to produce them, recent developments in energy storage facilities, and commitment of governments for the electrification of transportation. Although some limited recycling processes were developed earlier after the commercialization of LIBs, these are inadequate in the context of sustainable development. Therefore, significant efforts have been made to replace the commonly employed pyrometallurgical recycling method with a less detrimental approach, such as hydrometallurgical, in particular sulfate-based leaching, or direct recycling. Sulfate-based leaching is the only large-scale hydrometallurgical method currently used for recycling LIBs and serves as baseline for several pilot or demonstration projects currently under development. Conversely, most project and processes focus only on the recovery of Ni, Co, Mn, and less Li, and are wasting the iron phosphate originating from lithium iron phosphate (LFP) batteries. Although this battery type does not dominate the LIB market, its presence in the waste stream of LIBs causes some technical concerns that affect the profitability of current recycling processes. This review explores the current processes and alternative solutions to pyrometallurgy, including novel selective leaching processes or direct recycling approaches.

Recently, intensive efforts are dedicated to convert and store the solar energy in a single device. Herein, dye-synthesized solar cell technology is combined with lithium-ion materials to investigate light-assisted battery charging. In particular we report the direct photo-oxidation of lithium iron phosphate nanocrystals in the presence of a dye as a hybrid photo-cathode in a two-electrode system, with lithium metal as anode and lithium hexafluorophosphate in carbonate-based electrolyte; a configuration corresponding to lithium ion battery charging. Dye-sensitization generates electron–hole pairs with the holes aiding the delithiation of lithium iron phosphate at the cathode and electrons utilized in the formation of a solid electrolyte interface at the anode via oxygen reduction. Lithium iron phosphate acts effectively as a reversible redox agent for the regeneration of the dye. Our findings provide possibilities in advancing the design principles for photo-rechargeable lithium ion batteries.