A sustainable closed-loop approach for reclamation and reuse of graphite from end-of-life (EoL) lithium-ion batteries (LIBs) black mass is proposed. Low-impact froth flotation with green chemicals, followed by mild chemical purification and thermal treatment, is exploited. High-quality graphite is obtained. The direct recycling is validated through a closed-loop strategy from EoL to new cells, reusing the recovered material as regenerated anode.

The demand for lithium-ion batteries (LIBs) is posing challenges in the management of end-of-life (EoL) systems and supply of critical raw materials. Such challenges can be addressed by recycling EoL LIBs through sustainable processes, involving metallurgy to recover higher-value metals like Co, Ni, and Li. Pretreatment strategies allowing to reclaim other valuable materials—such as graphite, binders, and electrolytes—are also crucial to enhance the overall recycling efficiency. Despite the strategic relevance of graphite in the battery supply chain, its recovery and reuse remain poorly explored. Herein, a sustainable closed-loop approach for the reclamation and reuse of graphite from EoL LIBs black mass is proposed, exploiting a low-impact froth flotation based on green chemicals. The recovered graphite is purified through a mild chemical leaching by natural organic acids and thermally treated to restore its microstructure from damages induced by the aging phenomenon. The regenerated material is characterized by multi-sample technique approach, demonstrating high separation efficiency (>96% yield) and purity (>99.6%). The direct recycling process is validated by reusing the reclaimed graphite as secondary anode active material in new cells, showing functional performance comparable to those of the commercially available material.