High-Yield One-Pot Recovery and Characterization of Nanostructured Cobalt Oxalate from Spent Lithium-Ion Batteries and Successive Re-Synthesis of LiCoO2

Abstract

A complete recycling process for the cathode material of spent lithium-ion batteries is demonstrated with a simple two-step process comprised of one-pot cobalt recovery to nanostructured materials and single step synthesis of LiCoO 2 . For the facile and efficient recovery of cobalt, we employ malic acid as a leaching agent and oxalic acid as a precipitating agent, resulting in nanostructured cobalt oxalate. X-ray diffraction and Fourier transform infrared spectroscopy (FT-IR) analysis clearly show that cobalt species are simultaneously leached and precipitated as cobalt oxalate with a high yield of 99.28%, and this material can then be used as a reactant for the synthesis of LiCoO 2 for use as a cathode material. In addition to its advantages in simplifying the process, the proposed method allows for not only enhancing the efficiency of cobalt recovery, but also enabling reaction without a reducing agent, H 2 O 2 . Through successive single-step reaction of the obtained cobalt oxalate without any purification process, LiCoO 2 is also successfully synthesized. The effect of the annealing temperature during synthesis on the nanostructure and charge-discharge properties is also investigated. Half-cell tests with recycled LiCoO 2 exhibit a high discharge capacity (131 mA·h·g −1 ) and 93% charge-discharge efficiency.

A Fast Metals Recovery Method for the Synthesis of Lithium Nickel Cobalt Aluminum Oxide Material from Cathode Waste

“…The inorganic acids present a satisfactory performance during leaching and achieve higher efficiency of metal extraction than organic acids [29]. Techniques that are used to prepare the final products from the leaching filtrate include solvent extraction [10,[30][31][32][33], electrochemical techniques [34][35][36], selective precipitation [21,[37][38][39][40], and co-precipitation [41][42][43]. Among these, co-precipitation is the most efficient technique for the recovery of more than one metal (mixed metal) due to a higher level of homogeneity and spherical/sphere-like products [44].…”

Synthesis and Properties of Bulk Nanostructured Metallic Materials

“…Finally, five articles performed research on nanostructured materials for various functional and biomedical applications such as batteries, electronics, medicine, and high energy density reactants. Park et al [7] investigated a novel process that successfully recovered a nanostructured cathode from spent lithium-ion batteries and re-synthesized new cathode material. The author employed malic acid as a leaching agent and oxalic acid as a precipitating agent, resulting in the formation of nanostructured cobalt oxalate from which the new LiCoO 2 cathode was synthesized.…”

Recycling of cathode material from spent lithium-ion batteries

“…Park i sar. [111] su izvršili poređenje stepena efikasnosti izluženja Co upotrebom H 2 SO 4 i osam organskih kiselina (limunska, jabučna, malonska, askorbinska, akrilna, mlečna, sukcinska i tartarna kiselina). Rezultati eksperimenta ukazuju da je najveći stepen izluženja Co postignut upotrebom sumporne (95,80%), limunske (89,90%) i jabučne kiseline (86,69%).…”