Super concentrated HCl in a deep eutectic solvent as media for the integrated leaching and separation of metals from end-of-life lithium-ion batteries

abstract

Recycling spent lithium-ion batteries is vital to ensure the recovery of added-value resources and minimize environmental impact. Herein, an integrated and efficient process is developed for metal recovery from spent cathode powder combining both leaching and transition metal separation in one step. A hydrophobic deep eutectic solvent (DES) is proposed as a HCl super concentrator for the one-pot leaching of cathodes from spent lithium-ion batteries and simultaneous Ni(II) precipitation. The DES composed of decanoic acid and trioctylphosphine oxide can super concentrate HCl, 2.2-folds more than the aqueous limit of 37 wt%, whilst being thermally and chemically stable under leaching conditions up to 373 K. The proposed leaching process can quantitatively extract Co(II), Mn(II) and Cu(II) from spent cathodes of laptop batteries whilst only extracting 10 % of Ni(II). The latter could be easily recovered as NiCl2 center dot 2H(2)O with 99 % purity through the manipulation of the coordination environment afforded by the DES relative to aqueous media. Key leaching parameters were the HCl: metal molar ratio and temperature, both having a significant impact on the leaching efficiency and its selectivity. Metal recovery was accomplished after stripping of the loaded DES solution via a straightforward sequential precipitation process, with 99 % Co(II) and 98 % Mn(II) being precipitated with 95 % and 81 % purity, respectively. The reported system presents a better atom economy compared to other DES and conventional inorganic acids, providing a new mild approach for the simultaneous leaching and separation of metals from lithium-ion batteries.

keywords

HYDROMETALLURGICAL PROCESS; ACTIVE MATERIALS; VALUABLE METALS; REDUCING AGENT; RECOVERY; COBALT; OXIDE; EXTRACTION; ACIDS

subject category

Engineering

authors

Carreira, ARF; Nogueira, A; Crema, APS; Passos, H; Schaeffer, N; Coutinho, JAP

Groups

G4 - Renewable Materials and Circular Economy

Projects

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)

Collaboratory for Emerging Technologies, CoLab (EMERGING TECHNOLOGIES)

acknowledgements

This work was developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020, UIDP/50011/2020 & LA/P/0006/2020, financed by national funds through the FCT/MEC (PIDDAC) . Ana R. F. Carreira acknowledges FCT for the Ph.D. grant SFRH/BD/143612/2019. A.P.S. Crema acknowledges CAPES for the postdoctoral fellowship (88887.474466/2020-00). Nicolas Schaeffer acknowledges the national funds (OE) , through FCT-Fundacao para a Ciencia e a Tecnologia, I. P., in the scope of the framework contract foreseen in the numbers 4, 5, and 6 of the article 23, of the Decree-Law 57/2016, of August 29th, changed by Law 57/2017, of July 19th. Helena Passos acknowledges FCT - Fundacao para a Ciencia e a Tecnologia, I.P. for the researcher contract CEECIND/00831/2017 under the Scientific Employment Stimulus-Individual Call 2017. The authors thank Maria C.C. Azevedo and Marcia C. Neves for helping with Raman and SEM-EDS data acquisition, respectively.