Recycling Cathodes from Spent Lithium-Ion Batteries Based on the Selective Extraction of Lithium

Abstract

The demand for lithium-ion batteries (LIBs) has risen dramatically over the years. However, many of the essential component elements in cathodes, such as cobalt and lithium, are both costly with limited resources. Therefore, the recycling of spent LIB cathodes is of great significance to conserving resources and the environment. In this work, we reported a novel metal-based strategy to selectively leach lithium from different types of cathodes (NCM, LCO, and LMO) by Co2+ or Mn2+, which can realize over 95% lithium leaching rates without other metal ions, such as Ni2+, Co2+, and Mn2+, left in the leachate, and the residual transition metal oxides can be used as cathode precursors. Taking the spent LiCoO2 as an example, the regenerated LiCoO2 particles show decent electrochemical performance, i.e., a reversible discharge capacity of 137.9–162.5 mAh/g upon being charged to 4.2–4.4 V with excellent rate performance and cycling stability at 4.2 V. It is a facile, closed-loop, and scalable process for recycling spent LIB cathodes based on the preferentially selective extraction of lithium, which offers a novel strategy for recycling compositional Li-ion cathode materials.

Preferential Extraction of Lithium from Spent Cathodes and the Regeneration of Layered Oxides for Li/Na-Ion Batteries

“…As seen in Table S5, the lithium contents are further reduced from 0.52 to 0.01 during Stage II, while the ratio of M elements in R-200-18 has been restored to be the original value of S-NCM, which demonstrates the ion exchange reaction between Li + and M ions during Stage II. Our recent work has also confirmed that M 2+ can exchange with Li + from LiMO 2 following the charge balance principle under a M/Li ratio of 0.5 . In the case of stoichiometric H 2 SO 4 as the leaching reagent, part of Li + and M 2+ were first dissolved out from LiMO 2 by H + , while the released M 2+ would then exchange with the rest of the Li + from the remaining cathodes.…”

“…Our recent work has also confirmed that M 2+ can exchange with Li + from LiMO 2 following the charge balance principle under a M/ Li ratio of 0.5. 24 In the case of stoichiometric H 2 SO 4 as the leaching reagent, part of Li + and M 2+ were first dissolved out from LiMO 2 by H + , while the released M 2+ would then exchange with the rest of the Li + from the remaining cathodes. It is worth noting that the reactions involved are also subject to the charge balance principle, suggesting the selective extraction of Li + from LiMO 2 and formation of the MOOH phase under a H/Li ratio of 1.…”

Recovery of Li and Co from Spent Li-Ion Batteries by Mechanochemical Integration with NH4Cl

“…At the same time, waste LIBs are rich in lithium, cobalt and other resources, and their recycling is especially closed-loop. Recycling can alleviate environmental pollution while alleviating resource shortages. − Therefore, the closed-loop metal recycling technology for spent LCO batteries has received extensive attention …”

A sustainable strategy for spent Li-ion battery regeneration: microwave-hydrothermal relithiation complemented with anode-revived graphene to construct a LiFePO4/MWrGO cathode material

“…7 In contrast, cathodic LFP materials have the highest economic value, i.e., approximately 69% that of the whole battery. 8 However, the complex reclamation of Li salt from spent LFP through conventional hydrometallurgical treatments 9,10 based on combinations of leaching reagents (e.g., H 2 SO 4 or organic acid with H 2 O 2 ) 11,12 and precipitants (e.g., Na 2 CO 3 ) 13 hinders a 100% recovery, and it is also not economically or environmentally feasible enough to recycle because large quantities of chemical reagents and energy will be consumed for the resynthesis of new LFP cathodes. In summary, the lack of graphite recycling strategies and drawbacks of hydrometallurgy warrant a facile strategy that directly regenerates spent LFP cathodes and repurposes spent anodic graphite.…”

“…, approximately 69% that of the whole battery. 8 However, the complex reclamation of Li salt from spent LFP through conventional hydrometallurgical treatments 9,10 based on combinations of leaching reagents ( e.g. , H 2 SO 4 or organic acid with H 2 O 2 ) 11,12 and precipitants ( e.g.…”