Thermo-osmosis-Coupled Thermally Regenerative Electrochemical Cycle for Efficient Lithium Extraction

Lithium (Li) production based on the soda evaporation process is time-consuming and unsustainable. The emerging electrochemical Li extraction is time-efficient but requires high-concentration Li sources and significant electrical energy input. Here, we demonstrate a fast, energy-saving, and environment-friendly Li production process by coupling a thermally regenerative electrochemical cycle (TREC) using lithium manganese oxide (LMO) and nickel hexacyanoferrate (NiHCF) electrodes with poly(vinylidene fluoride) membrane-based thermo-osmosis (denoted as TO-TREC). The characterization of LMO and NiHCF electrodes confirmed that the relatively high temperature of TO-TREC has negligible adverse effects on the ion intercalation in LMO and NiHCF electrodes. The LMO/NiHCF pair has a positive temperature coefficient of 0.843 mV K^-1. In the TO-TREC process, Li ions are selectively extracted from a Li-containing brine warmed by low-grade heat and then released into a room-temperature recovery solution such as LiCl with a production rate of 50-60 mmol Li⁺ m^-2 h^-1. Li source solutions are concentrated by thermo-osmosis simultaneously, making it possible to utilize previously unusable Li-containing sources, such as concentrated brines from desalination plants and industrial effluents. Besides, the TREC harvests thermal energy from the heated brine, saving >20% of electrical energy compared to conventional electrochemical methods. The new process shows the potential to meet the growing global Li demands for many applications.