Pollutant-free pyrolysis strategy for direct upgrading of cathode materials from spent lithium-ion batteries

Abstract

The recycling of lithium-ion batteries (LIBs) has been dogged by air pollutants containing fluoride (e.g. HF, PF₅, POF₃). Pyrolysis is a technique that can eliminate polyvinylidene fluoride (PVDF) from the cathode electrode sheets of spent LIBs, effectively separating the cathode material from the aluminum (Al) foil. Nonetheless, the HF gas generated during pyrolysis not only corrodes equipment but also presents serious environmental risks. To address this, a novel, eco-friendly strategy is introduced for the direct upgrading of cathode active materials (CAM). The strategy's cornerstone involves incorporating a minor amount of calcium into the original cathode material's coating, and it leverages mechanical stirring during the waste battery material separation process to ensure the electrode is fully detached from the current collector at a reduced temperature. The pyrolysis mechanism elucidates that fluorine-containing organic pollutants are converted into metal fluorides and deposited on the surface of cathode particles during aerobic pyrolysis, thereby improving the interfacial stability of lithium nickel cobalt manganese oxide (NCM) materials, reducing transition metal dissolution. This strategy not only eliminates the release of fluorine-containing organic pollutants during pyrolysis but also achieves direct regeneration of CAM. This work underscores the importance of the cathode materials' manufacturing process in facilitating the recycling of spent LIBs and provides an environmentally friendly and economically viable solution for the battery recycling industry.