Abstract

With the substantial increase in the demand for lithium-ion batteries (LIBs) for the adoption of electrification to reduce CO2 emission, safe and efficient recycling of spent LIBs is essential to utilize LIBs sustainably1. In hydrometallurgy-based or direct LIB recycling systems, which are expected to become mainstream in the future because of their low environmental impacts, deactivation is a crucial pretreatment step to safely handle LIBs during the processes2, 3. However, a common deactivation method, in which an external short circuit is induced using electronic loads or conductive liquid, cannot deactivate LIBs with disconnected electrical circuits or metallic Li plating on the negative electrode surface, despite their high safety risks.We propose the advanced deactivation method, injecting a redox mediator (RM) solution inside the LIBs. The RM delivers electrons from the negative electrode to the positive electrode by cycling the reduction and oxidation on the negative and positive electrodes, respectively (redox shuttle reaction), resulting in discharging LIBs. In other words, the RM causes a short circuit inside the LIB. Therefore, it is possible to discharge a LIB that cannot be discharged externally, for example, a LIB with disconnected electrical circuits due to a safety device operation. Furthermore, the RM can strip Li metal plated on the negative electrode even though it is “dead lithium.” This unique characteristic contributes to the improvement in the safety and the Li collection rate in the recycling processes. Additionally, in this presentation, the deactivation mechanism of LIBs and its relationship with the electrochemical properties of the RMs will be discussed. The present findings will be beneficial and helpful for designing RMs for deactivation of more and more diversified spent LIBs. References J. Neumann, et al.: "Recycling of Lithium‐Ion Batteries—Current State of the Art, Circular Economy, and Next Generation Recycling" Adv. Energy Mater. 12, (2022). A. Kwade, et al.: "Recycling of lithium-ion batteries" The LithoRec Way, Switzerland: Springler International Publishing AG (2018). H. Rouhi, et al.: "Voltage behavior in lithium-ion batteries after electrochemical discharge and its implications on the safety of recycling processes" Journal of Energy Storage 35, (2021).

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