ABSTRACT Sustainable recovery of lithium from salt lake brines is essential for the transition toward clean energy but remains challenged by low Li + concentrations and high Mg 2+ interference. Herein, we develop a heterostructure‐engineered ternary composite, conductive metal‐organic frameworks (c‐MOFs) coupled with a MoSe 2 @MXene framework for efficient and selective lithium extraction by capacitive deionization (CDI) technology. The c‐MOFs Fe‐ tetrahydroxybenzoquinone (Fe‐THBQ) provide abundant redox‐active sites for Li⁺ capture, while the MoSe 2 @MXene framework accelerates ion transport rate and provides structural robustness. X‐ray absorption spectroscopy (XAS) confirms that strong interfacial Fe─Se coordination bonds establish a continuous Fe‐Se‐Mo charge‐transfer pathway for enhanced conductivity and ion selectivity. Thus, the Fe‐THBQ@MoSe 2 @MXene electrode delivers exceptional Li⁺ capture capacity (4.05 mmol g −1 ), ultrafast adsorption rate (0.98 mmol g −1 min −1 ), superior cycling stability (91.3% retention after 50 cycles), and remarkable Li⁺ selectivity with high Mg/Li ratios in both model solutions and real Dachaidan salt lake brine. Ex situ X‐ray diffraction analyses reveal a dual Li + storage mechanism involving Fe 2+ /Fe 3+ redox activity and reversible interlayer intercalation. Importantly, density functional theory (DFT) calculations confirm a substantially lower migration barrier for Li⁺ (0.052 eV) compared to competing cations, underpinning the observed selectivity. This work highlights a rational heterostructure design strategy for advancing CDI technology in lithium recovery.
Li et al. (Sun,) studied this question.