Selective Copper Removal from an Fe-P-Cu Alloy Recovered by Pyrometallurgical Reduction of Spent LiFePO₄ Batteries...

The recycling of spent lithium iron phosphate (LiFePO₄, LFP) batteries is receiving increasing attention as electric-vehicle deployment accelerates worldwide. Pyrometallurgical reduction offers a viable route for large-scale recovery of iron-rich products from spent LFP batteries; however, the resulting Fe-based alloys often retain residual copper (Cu), which deteriorates alloy quality and constrains downstream utilization and refining. In this study, a sulfidation-slag refining process was developed to selectively remove Cu from an Fe-P-Cu alloy produced by dry reduction of spent LFP batteries. FeS was employed as a sulfidizing agent to promote preferential conversion of Cu into sulfide phases, while fayalite (Fe₂SiO₄) slag was introduced to enhance phase separation between metallic and sulfide/slag phases. Thermodynamic calculations coupled with high-temperature experiments were conducted at 1400-1600 °C under various Cu:FeS ratios to identify operating conditions that maximize Cu removal while minimizing Fe loss. The results indicate that Cu is selectively transferred from the metallic phase to Cu-Fe-S sulfide phases, whereas Fe remains predominantly in the metal phase. Under the optimal condition (1400 °C, Cu:FeS = 2:1), the refined metal reached an Fe content of 90.80 wt.%, achieving an Fe recovery of 87.42% and a Cu removal efficiency of 81.13%. The proposed approach provides a practical stepwise refining strategy for upgrading Fe-rich secondary resources recovered from spent LFP batteries and facilitates subsequent impurity-control processes.