Efficient and cost-effective recycling of spent lithium-ion batteries is essential for the sustainable growth of the clean energy sector, conserves critical mineral resources, and contribute to environmental sustainability. The pyrometallurgy process, involving high-temperature smelting and solid-state reduction, plays a key role in the industrial-scale recycling of these batteries. Traditional smelting methods, however, face criticism for their substantial energy requirements and the loss of lithium in slag. In this study, an innovative laser-based in-situ pyrometallurgical process, hereinafter referred to as laser recycling, was developed to recycle Li-ion batterie materials without using slag, enabling the simultaneous recovery of Co, Ni, Mn, and Li. Lab-scale experiments were carried out to investigate the influences of laser power density and duration on the carbothermic reduction behavior of battery materials. The results showed that the maximum temperature reached approximately 1850 °C with a laser power between 1500 and 2000 W focused to an area of 20 mm in diameter within a few seconds. The laser recycling facilitates concurrent smelting and solid-state reduction, with carbothermic reduction completed in just 30 s due to rapid reaction kinetics, ultra-high temperatures, and the enhanced contact area resulting from surface tension-driven molten material flow under intense laser beam exposure. This laser recycling process reduced LiCoO2 and LiNi0.33Mn0.33Co0.33O2 to metallic Co or Co-Ni-Mn alloy, respectively, while Li was recovered as Li2CO3. The new process allowed for the near-total recovery of Co, Ni, and Mn in the alloy and virtually 100% Li recovery in the form of Li2CO3 by a vapor phase capture system. Additionally, continuous laser recycling in the battery material powder bed showed potentials to scale up for industry battery recycling. A mechanism for the laser recycling process was proposed. A preliminary discussion on the techno-economic implications of laser recycling was also provided.
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