Direct Recycling Technology for Spent Lithium-Ion Batteries: Limitations of Current Implementation

The significant deployment of lithium-ion batteries (LIBs) within a wide application field covering small consumer electronics, light and heavy means of transport, such as e-bikes, e-scooters, and electric vehicles (EVs), or energy storage stationary systems will inevitably lead to generating notable amounts of spent batteries in the coming years. Considering the environmental perspective, material resource sustainability, and terms of the circular economy, recycling represents a highly prospective strategy for LIB end-of-life (EOL) management. In contrast with traditional, large-scale, implemented recycling methods, such as pyrometallurgy or hydrometallurgy, direct recycling technology constitutes a promising solution for LIB EOL treatment with outstanding environmental benefits, including reduction of energy consumption and emission footprint, and weighty economic viability. This work comprehensively assesses the limitations and challenges of state-of-the-art, implemented direct recycling methods for spent LIB cathode and anode material treatment. The introduced approaches include solid-state sintering, electrochemical relithiation in organic and aqueous electrolytes, and ionothermal, solution, and eutectic relithiation methods. Since most direct recycling techniques are still being developed and implemented primarily on a laboratory scale, this review identifies and discusses potential areas for optimization to facilitate forthcoming large-scale industrial implementation.