Closed-loop recycling of spent lithium-ion batteries based on selective sulfidation: An unconventional approach

Abstract

The facile recycling of spent lithium-ion batteries (LIBs) has attracted considerable attention because of its great importance to environmental protection and resource utilization. A novel process is developed for cyclic utilization of spent LiNi_xCo_yMn_zO₂ (NCM) batteries. The spent NCM was converted into water-soluble Li₂CO₃, acid-dissolved MnO, and nickel-cobalt sulfides through selective sulfidation, based on roasting condition optimization and thermodynamic calculation. More than 98 % of lithium is extracted preferentially from calcined NCM through water leaching, and over 99 % of manganese is extracted selectively from water leaching residue with H₂SO₄ solution of 0.4 mol/L in the absence of additional reductant. The nickel and cobalt sulfides were concentrated into the leaching residue without metal impurities. The obtained Li₂CO₃, MnSO₄, and nickel-cobalt sulfides can be regenerated as new NCM, showing good electrochemical performance, and its discharge capacity is 169.8 mAh/g at 0.2C. After 100 cycles at 0.2C, the discharge specific capacity can still be maintained at 143.24 mAh/g, and its capacity retention ratio is as high as 92 %. An environmental assessment and economic evaluation indicate that the process is an economical and eco-friendly approach for green recycling of spent LIBs.

Keywords: Circular economy; Hazardous solid waste; Regeneration of cathode material; Selective sulfidation; Spent lithium battery; Water leaching.