Harnessing Faradaic Deionization in Battery Recycling: Challenges of using inorganic electrode materials for lithium recovery
RAQUEL CASASOLA FERNÁNDEZ a, ALBA FOMBONA-PASCUAL a, ENRIQUE GARCÍA-QUISMONDO HERRÁIZ a, JESÚS PALMA DEL VAL a, JULIO LADO GARRIDO a
a IMDEA ENERGIA
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Electrochemical Water Treatment - #ELECTROWAT
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Julio J. Lado and Ignacio Sirés Sadornil
Oral, RAQUEL CASASOLA FERNÁNDEZ, presentation 293
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.293
Publication date: 16th December 2024

Pyrometallurgy is one of the most relevant processes to recycle Lithium-ion Batteries (LIB). It involves the melting of the waste batteries in a shaft furnace at around 1500ºC. Two main products are obtained: an alloy, rich in Ni, Co, Cu, Fe; and a slag, which mainly contains Li and Al [1]. Typically, this slag was not valorised, and its main application was as a filling material in the construction sector. In 2021, one of the main European companies in the field of battery recycling published a patent where they claim a hydrometallurgical process to recover lithium from this slag, by leaching with H2SO4 and then precipitating Al to leave Li in solution [2]. The present study arose as an attempt to investigate the possibility of lithium extraction from leaching solutions containing aluminium.

Our approach focuses on exploring electrochemical capture technologies, such as faradaic deionization, to minimize the chemical usage and provide a more cost-effective, energy-efficient and environmentally sustainable solution. For that purpose, various lithium metal oxides (LMO, LFP, LMFP, NMC) were tested as active materials for electrochemical lithium recovery. Lithium manganese oxide (LMO) emerges as a promising candidate leading to the synthesis of Truncated-Octahedral LMO (Tr-Oh-LMO) [3], theoretically more stable than commercial LMO, to enhance the robustness of the process. Electrodes were prepared in two configurations, carbon paper (CP) and buckypaper (BP), and tested across different electrolyte compositions and pH values.To assess the performance, a novel Electrode Endurance Diagram was proposed to visualize the influence of pH on electrode stability during cycling. This tool enables a quick and comparative evaluation of the performance of different materials across a range of pH levels. Additionally, various characterization techniques, such as XRD and SEM-EDS, are employed to investigate electrode degradation mechanisms as a function of pH and aluminum presence.

Overall, this work provides valuable insights into the influence of pH and aluminum on the stability of lithium oxide electrodes, emphasizing the need to optimize process conditions and explore alternative active materials to enhance the feasibility of electrochemical lithium extraction from aluminum-rich solutions.

This research was supported by the Comunidad de Madrid through the Talent Attraction Program (SELECTVALUE, 2020-T1/AMB-19799, PI J.L.) and by the Grant PID2023-153183OA-I00 (NET4BAT), funded by MICIU/AEI/10.13039/501100011033 and by ERDF/EU. RC also gratefully acknowledges support from the María de Maeztu Unit of Excellence grant. The authors wish to extend their thanks to Irene Hormigos for her collaboration in the laboratory experiments.

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