Li₂CO₃ Recovery through a Carbon-Negative Electrodialysis of Lithium-Ion Battery Leachates

Abstract

Recycling of lithium-ion batteries (LIB) has focused on the recovery of metals such as Co and Ni due to their intrinsic values. Among these metals, recycling of Li requires hydrometallurgical routes that are not widely implemented due to the higher costs associated with energy and chemical consumptions. This makes Li recovery from recycling less economical than obtention from mineral ores. In the present study, Li as well as Mn were recovered through electrodialysis (ED) from the leachates of spent LIBs by employing a CO 2 -capture agent N-methyldiethanolamine as a regenerable catholyte. Surrogate solutions and Li-rich leachates were tested for the separation and recovery of Li and Mn as Li 2 CO 3 and MnCO 3 , respectively. The purity of recovered Li 2 CO 3 99.6% achieved battery-grade purity levels from both surrogate and leachate solutions. It was observed that MnO 2 was deposited on the Pt anode only from the surrogate solutions. Energy consumption of the ED was low at 0.5 kW h/g Li. The overall process recovered high-purity Li from LIB leachate, with CO 2 being the only chemical consumed. This process is presented as an environment-friendly and energy-effective method in Li 2 CO 3 recovery from LIB materials.

Electrochemical Approach for Lithium Recovery from Spent Lithium-Ion Batteries: Opportunities and Challenges

“…Lithium ions pass through the monovalent cation exchange membrane, react with CO 2 in the catholyte, and precipitate as Li 2 CO 3 , with a purity of 99.60% and a yield of 48.4%. 90 The presence of Mn in the catholyte indicated the permeability of Mn through this monovalent ion exchange membrane. 90 The monovalent ion exchange membraneassisted electrodialysis process is a promising and straightforward method to recover lithium from the LIB leachate.…”

Carbon dioxide utilization in lithium carbonate precipitation: A short review

“…The research conducted by Meng Shi focused on a unique electrodialysis (ED) method for recovering Li and manganese from spent LiBs [58]. Unlike the hydrometallurgical routes traditionally used for Li recycling, this study used electrodialysis (ED), employing a CO 2 -capture agent, N-methyldiethanolamine, as a regenerable catholyte.…”

Sustainable Lithium Recovery from Hypersaline Salt-Lakes by Selective Electrodialysis: Transport and Thermodynamics

“…31,36 As illustrated in Figure 1, the composite CEM acquires a positive zeta potential and exhibits passive selectivity for monovalent cations from the enhanced Donnan exclusion effect. 4,29 Based on experiments with dilute binary cation solutions, selectivity enhancements in Li + /Mg 2+ separations with multilayered or polyelectrolyte ion-exchange membranes are well documented in the literature. 4,31,32,43−45 As stressed in recent reviews on salt-lake lithium extraction, however, over 95% of prior work disregards the deleterious impacts from competing ions and the high feed salinity that is representative of salt-lake brines.…”

“…Further, by avoiding brine evaporation altogether, DLE can be viable for dilute lithium sources . The high Mg 2+ concentrations in salt-lake brines, however, attenuate the extraction effectiveness of DLE, as a result of the comparable solubility products and ionic radii of Li + and Mg 2+ . ,, DLE methods to isolate Li from a Na-rich mixture typically require the Li + /Mg 2+ ratio of the brine to be greater than approximately 4 to minimize chemical usage for precipitation and/or solvent recovery. , To enhance the selectivity and the atomic efficiency of DLE, the salt-lake brine can be pretreated with membrane processes like nanofiltration (NF) − or electrodialysis (ED) − to eliminate multivalent cations. The prospect of ED for lithium concentration from salt-lakes is particularly promising because of its successful commercial history in salt production from hypersaline brines. , …”

“…In an electrodialysis module, cation- and anion-exchange membranes (CEM and AEM, respectively) are arranged in an alternating order between two electrodes, separating the feed stream into diluate and concentrate product streams. , Conventional CEMs and AEMs are monopolar water-swollen polymeric films that typically contain negatively charged perfluorosulfonic acid and positively charged quarternary ammonium moieties, respectively . As a result of the charged moieties, the electrostatic potentials that form along the solution-membrane interface inhibit ions of the same charge (i.e., co-ions) from partitioning into the interstitial phase of the membrane, − a phenomenon known as Donnan exclusion. , To impart monovalent cation selectivity, , typically a thin polyethylenimine (PEI) surface layer is covalently bonded with the CEM substrate through a condensation reaction between the perfluorosulfonic acid and amine moieties. , As illustrated in Figure , the composite CEM acquires a positive zeta potential and exhibits passive selectivity for monovalent cations from the enhanced Donnan exclusion effect. , …”