Peer-reviewed publication: Direct Synthesis of Li-Mn-Rich Cathode Precursor from End-of-Life Li-Ion Batteries
Peer-reviewed publication: Direct Synthesis of Li-Mn-Rich Cathode Precursor from End-of-Life Li-Ion Batteries
04/09/2025
Authors: Ludovica D’Annibale, Pier Giorgio Schiavi, Arcangelo Celeste, Sergio Brutti, Francesca Pagnanelli, Pietro Altimari
Department of chemistry, University La Sapienza of Rome, Italy
An innovative hydrometallurgical process is analysed, enabling the direct synthesis of graphene oxide and lithium-manganese rich cathode materials from the electrodic powder (“black mass”) of spent lithium-ion batteries. The black mass leaching is performed by the Hummers’ method, an established solution to produce graphene oxide from graphite. The proposed strategy is based on the the observation that the reagents H2SO4 and H2O2, which are conventionally used to perform the leaching of the black mass, are also used, along with
KMnO4 and NaNO3, in the implementation of the Hummers’ method. Accordingly, the Hummers’ method is here carried out to extract the cathode metals from the black mass (Li, Mn, Co, Ni). To valorise the manganese excess generated by the addition of KMnO4, co-precipitation from the residual solution obtained after graphene oxide recovery is carried out to synthesize the precursor of the lithium-manganese rich cathode materials, which is then used to produce the cathode material by solid-state reaction with LiOH. In this contribution, an experimental analysis of this resynthesis process is presented, allowing to evaluate the impact of the main process parameters on the precursor material synthesis. The proposed process includes the removal of impurities such as copper, iron, and aluminium, followed by the coprecipitation of a precursor with the composition Ni0.375Mn1.375Co0.25(OH)2.
