Ultrafast recycling of spent lithium-ion batteries via laser-induced carbothermal reduction with synergistic regulation ofmicro-morphology and lattice defects

Efficient recycling of spent lithium-ion batteries (LIBs) is pivotal for mitigating the looming shortage of critical metals and the environmental burden posed by the massive accumulation of battery waste. However, conventional pyrometallurgical and hydrometallurgical processes are often constrained by their reliance on inert atmospheres and sluggish leaching kinetics. Herein, we propose a Laser-induced Carbothermal Reduction (LCTR) strategy for the low-carbon recovery of spent cathodes and demonstrate a synergistic mechanism that couples micro-morphological restructuring with lattice defect engineering. Laser-induced transient thermal shock triggers the stress-driven pulverization of secondary particles, increasing the specific surface area, while simultaneously reducing high-valence transition metals and generating oxygen vacancies. This dual modification enables rapid dissolution kinetics (15 min) in mild acid (0.5 M H₂SO₄), achieving a lithium recovery rate of 99.72% and >90% for transition metals. Furthermore, the process exhibits broad universality across diverse cathode chemistries (including NCM series, LiCoO₂, and LiMn₂O₄) and authentic spent electrodes. This study not only elucidates the microscopic mechanisms of laser-matter interaction but also presents a high-throughput, economically viable paradigm for sustainable urban mining.