Multifunctional Scavenger Boosts Cathode Interfacial Stability with Reduced Water Footprint for Direct Recycling of Spent Lithium‐Ion Batteries

Abstract The burgeoning accumulation of spent lithium‐ion batteries (LIBs), a byproduct from the widespread adoption of portable electronics and electric vehicles, necessitates efficient recycling strategies. Direct recycling represents a promising strategy to maximize the value of LIB waste and minimize harmful environmental outcomes. However, current efforts to large‐scale direct recycling face challenges stemming from heterophase residues (e.g., Li₂CO₃, LiOH) in the recycled products and uncontrolled interfacial instability, often requiring repeated washing that generates significant wastewater. Here, a refined direct recycling process is proposed to improve cathode interface stability by leveraging in situ reaction between surface residual lithium species and a weak inorganic acid to form a conformal Li⁺ conductive coating that stabilizes the regenerated Ni‐rich cathodes with significantly reduced water footprint. The findings reveal that the conductive coating also prevents direct contact between contaminants and the cathode surface, thus improving the ambient storage stability. By eliminating the need for extensive washing, this intensified recycling process offers a more sustainable approach with the potential to transition from laboratory to industrial‐scale applications, improving both product quality and environmental sustainability.