A promising selective recovery process of valuable metals from spent lithium ion batteries via reduction roasting and ammonia leaching

Abstract

In this study, a promising process has been developed for selective recovery of valuable metals from spent lithium ion batteries (LIBs). First, reduction roasting which used spent anode powder as reduction agent and water immersion are applied to preferentially recover lithium. Subsequently, an ammonia leaching method is adopted to eff ;ectively separate nickel and cobalt from water immersion residue. Results indicate that Li₂CO₃, (NiO)_m·(MnO)_n, Ni, Co are the ultimate reduction products at 650 °C for 1 h with 5% anode powder. 82.2 % Li is preferentially leached via water immersion after reduction roasting and Li₂CO₃ products are obtained by evaporation crystallization. Thermodynamics shows that reducing ammonia leaching is feasible for water immersion residue. Amounts of 97.7 % Ni and 99.1 % Co can be selectively leached by NH_3·H₂O and (NH₄)₂SO₃ while Mn remain in the residue as (NH₄)₂Mn(SO₃)_2·H₂O, (NH₄)₂Mn(SO₄)_2·6H₂O and (NH₄)₂Mn₂(SO₃)₃ under the optimized conditions. Ammonia leaching kinetic show the activation energy of Ni and Co is 84.44 kJ/mol and 91.73 kJ/mol, which indicate the controlling steps are the chemical reaction. Summarily, the whole process achieves the maximum degree of selective recovery and reduces the environmental pollution caused by the multistep purification.

Keywords: Ammonia leaching; Reduction roasting; Selective recovery; Spent LIBs; Water immersion.