Sustainable recycling of spent lithium-ion batteries via spontaneous chemical delithiation

Abstract

The rapid growth of portable electronics and electric vehicles has increased the demand for lithium-ion batteries (LIBs), raising concerns about spent LIBs and their recycling methods. Conventional recycling methods face limitations due to complex procedures, high energy consumption, and environmental hazards. Herein, we present a simple and scalable pre-lithium extraction (PLE) process for extracting lithium and recovering battery components from charged spent LIBs. The PLE process selectively extracts lithium from lithiated graphite in anode of charged LIBs using an aqueous lithium extraction solution under mild conditions, without crushing, heat treatment, and acid leaching. By incorporating of isopropyl alcohol into the lithium extraction solution, the vigorous reaction between the charged LIBs anode and water suppressed, resulting in the safe recovery of lithium. In a 60 Ah Li-NCM cell test, 93 % of lithium was recovered as Li2CO3 with 99.4 % purity. The PLE process also demonstrates both universality and scalability, being successfully applied to various types of LIBs and at the pilot scale. Furthermore, this new process significantly reduces energy consumption and greenhouse gas (GHG) emissions compared to conventional recycling methods, underscoring its strong environmental and industrial potential. This new process presents a promising pathway toward industrial-scale LIB recycling and a closed-loop battery economy.