Research on the recycling of waste lithium battery electrode materials using ammonium sulfate roasting

Abstract

Owing to resource limitations, environmental pollution concerns, and the increasing global demand for lithium-ion battery raw materials, the recycling of discarded electrode materials from lithium-ion batteries has emerged as a prominent research area. Nevertheless, among various types of discarded lithium battery electrode materials, limited research has been conducted on the recycling of ternary electrode materials (LiNixCoyMn1-x-yO2). This study proposes an eco-friendly process for the efficient recovery of valuable metals and carbon from mixed materials of discarded ternary lithium-ion battery electrodes. This study investigated the influence of various roasting using ammonium sulfate and leaching conditions on the conversion and extraction rates of valuable metals. Under the condition of a 3:1 mass ratio of ammonium sulfate to lithium battery electrode mixed material, roasting temperature of 450 °C, roasting time of 30 min, liquid-solid ratio of 20:1, leaching time of 20 min, and leaching temperature of 60 °C, the recovery rates of various valuable metals including Li, Ni, Co, and Mn reached 99.99%. For the above process, the chemical control reaction prevailed in the initial 10 min of the roasting reaction, succeeded by the dominance of diffusion control reaction in the subsequent 20 min. In the leaching process, the chemical control reaction governed the first 2 min, succeeded by diffusion control reaction for the next 18 min. Analysis of the reaction's macroscopic and microscopic mechanisms reveals that ammonium sulfate roasting of waste ternary lithium-ion batteries constitutes a typical liquid-solid reaction. In the molten state, NH4+ decomposition releases high-energy H+ ions that break the bonds between metals and oxygen. Consequently, metal atoms from the waste battery's crystal structure combine with ammonium sulfate's sulfate groups, forming various metal sulfates. This paper establishes an eco-friendly process for the efficient recovery of valuable metals by employing the ammonium sulfate roasting method to convert valuable metals in discarded electrode mixed materials into water-soluble sulfates.