Ultrafast Recycling of Spent Lithium-ion Batteries via Laser-induced Carbothermal Reduction with Synergistic Regulation of Micro-morphology and Lattice Defects

Abstract

Efficient recycling of spent lithium-ion batteries is pivotal for addressing the looming shortage of critical metals and the environmental burden caused by the massive influx 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 fragmentation with lattice defect engineering. Laser-induced transient thermal shock triggers the stress-driven pulverization of secondary particles, significantly 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.