Highly efficient recovery of waste LiNi_xCo_yMn_zO₂ cathode materials using a process involving pyrometallurgy and hydrometallurgy

Abstract

● A gentle series process is proposed to gradually leach valuable metals.

● Approximately 87% Li, 97.01% Co, 97.08% Ni and 99% Mn can be leached.

● The mechanism of LiNi _x Co _y Mn _z O₂ decomposition during reduction roasting is elucidated.

● Li₂CO₃, CoSO₄, NiSO₄ and MnSO₄ are successfully recovered.

Substantial environmental and economic benefits can be achieved by recycling used lithium-ion batteries. Hydrometallurgy is often employed to recover waste LiNi_xCo_yMn_zO₂ cathode materials. As Ni, Co and Mn are transition metals, they exhibit similar properties; therefore, separating them is difficult. Thus, most researchers have focused on leaching processes, while minimal attention has been devoted to the separation of valuable metals from waste LiNi_xCo_yMn_zO₂ cathode materials. Herein, we propose an environment-friendly, gentle process involving the usage of pyrometallurgy and hydrometallurgy to gradually leach valuable metals and effectively separate them. Interestingly, Li is recovered through a reduction roasting and water leaching process using natural graphite powder, Ni and Co are recovered through ammonia leaching and extraction processes and Mn is recovered through acid leaching and evaporation–crystallization processes. Results show that ~87% Li, 97.01% Co, 97.08% Ni and 99% Mn can be leached using water, ammonia and acid leaching processes. The result obtained using the response surface methodology shows that the concentration of (NH₄)₂SO₃ is a notable factor affecting the leaching of transition metals. Under optimal conditions, ~97.01% Co, 97.08% Ni and 0.64% Mn can be leached out. The decomposition of LiNi_xCo_yMn_zO₂ is a two-step process. This study provides valuable insights to develop an environment-friendly, gentle leaching process for efficiently recycling valuable metals, which is vital for the lithium-ion battery recycling industry.

Graphical abstract

Keywords

Waste LiNi _xCo _yMn _zO ₂ cathode materials / Leaching / Effective separation / Series process

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