Interlayer-Tailored Alkyl-MXenes for Selective Electrochemical Lithium-Ion Extraction

Abstract

The efficient and selective extraction of lithium ions from aqueous media is crucial for resource recovery, yet remains challenging due to the chemical similarity of coexisting alkali ions, such as sodium. In this study, we report a two-step electrochemical strategy that utilizes tailored MXene electrodes for lithium ion extraction with enhanced selectivity and extraction rates. By preintercalating hexadecylamine (HDA) and decyltrimethylammonium (C10), which are long-chain organic molecules, into the Ti3C2Tx MXene structure, we tailored the interlayer environment to favor lithium ions over sodium ions. The HDA-intercalated MXene demonstrated high Li+/Na+ selectivity with a lithium ion uptake of 2.2 mmol/L and a suppressed sodium ion uptake (<0.2 mmol/L). Extended cycling revealed that molecular preintercalation modulates ion transport pathways and influences structural and electrochemical stability. Both HDA-Ti3C2Tx and C10-Ti3C2Tx maintained a lithium ion purity of nearly 100% over 50 cycles.