Universal and efficient extraction of lithium for lithium-ion battery recycling using mechanochemistry

Abstract

The increasing lithium-ion battery production calls for profitable and ecologically benign technologies for their recycling. Unfortunately, all used recycling technologies are always associated with large energy consumption and utilization of corrosive reagents, which creates a risk to the environment. Herein we report a highly efficient mechanochemically induced acid-free process for recycling Li from cathode materials of different chemistries such as LiCoO2, LiMn2O4, Li(CoNiMn)O2, and LiFePO4. The introduced technology uses Al as a reducing agent in the mechanochemical reaction. Two different processes have been developed to regenerate lithium and transform it into pure Li2CO3. The mechanisms of mechanochemical transformation, aqueous leaching, and lithium purification were investigated. The presented technology achieves a recovery rate for Li of up to 70% without applying any corrosive leachates or utilizing high temperatures. The key innovation is that the regeneration of lithium was successfully performed for all relevant cathode chemistries, including their mixture.

Interfacial process engineering of a co-grinding agent for recycling spent lithium-ion batteries

“…The XPS spectra of Li 1s show the presence of LiAlO 2 . From these observations, it can be inferred that Al participates in the reduction of Co 3+ (as shown in eqn (4)–(6)), 38 and the generated AlF 3 can effectively reduce the contamination of Al 3+ on the recovered products. The XPS spectra of C 1s indicate that after milling for 30 min, the relative CO 3 2− content increases while the relative C–C (graphite) content decreases (Table S4†).…”

“…However, the drawback of this method is the long milling time, and recovery methods for other valuable metals from the solid-phase extraction residue have not yet been explored. Similarly, using reducible substances like iron powder, 30 aluminum powder 38 and copper powder 39 as co-grinding agents can reduce cobalt from the trivalent to divalent state, expediting the leaching. Nevertheless, the challenge lies in the subsequent separation and purification, which becomes more complex due to the presence of metal reducing agents.…”

The InnoRec Process: A Comparative Study of Three Mainstream Routes for Spent Lithium-ion Battery Recycling Based on the Same Feedstock

“…Other approaches to the processing of recycling intermediates are increasingly looking at the use of mechanochemical reactions in grinding media mills. For example, cathode active materials are processed together with reducing agents to catalyze a reaction of lithium metal oxides to lithium aluminate [47]. However, corresponding process steps are not considered in the present study.…”

Revealing the mechanism of reductive, mechanochemical Li recycling from LiFePO4

“…Past research has documented the use of ball-milling with Al as a co-grinding agent to induce reductive mechanochemical reactions, aiming to extract valuable elements from various cathode materials in an environmentally friendly and straightforward manner. 34,39 Importantly, when Al is used as a reducing agent, removing the Al cathodic current collector is unnecessary, as it can be repurposed in the reaction, further simplifying the overall recycling process. While this recycling approach has proven to be very effective for various cathode materials, it has only achieved low lithium recovery rates when applied to LFP.…”