Laser‐Induced Regeneration of Spent LiMn2O4 Cathode Into High‐Performance Ni‐Doped LiMn2O4 Cathode

Abstract The rapid increase in lithium‐ion battery (LIB) production, fueled by the rise of electric vehicles, highlights significant challenges in managing end‐of‐life LIBs, particularly regarding environmental impact and waste management. Traditional recycling methods, such as pyrometallurgical and hydrometallurgical processes, are energy‐intensive and consume substantial reagents. In this study, a laser‐assisted regeneration method is introduced for LiMn 2 O 4 (LMO) cathodes, enabling in situ Ni doping into spent LMO cathodes (r‐LMO‐Ni) to enhance electrochemical performance. Surface Ni‐doping improves interfacial processes and reduces capacity loss at lower temperatures by creating a new interface with a lower charge transfer energy barrier. The r‐LMO‐Ni cathode surpasses pristine LMO cathodes, achieving a specific capacity of 112.95 mA h g −1 at 1 C and retaining 95.1% of its capacity after 200 cycles at 0 °C. A techno‐economic analysis supports the feasibility of this laser‐assisted regeneration approach, offering an innovative pathway for upcycling spent cathodes and developing next‐generation Mn‐based cathodes.