MXene/Activated-Carbon Hybrid Capacitive Deionization for Permselective Ion Removal at Low and High Salinity

Two-dimensional, layered transition metal carbides (MXenes) are an intriguing class of intercalation-type electrodes for electrochemical applications. The ability for preferred counterion uptake qualifies MXenes as an attractive material for electrochemical desalination. Our work explores Ti3C2Tx-MXene paired with activated carbon in such a way that both electrodes operate in an optimized potential range. This is accomplished by electrode mass balancing and control over the cell voltage. Thereby, we enable effective remediation of saline media with low (brackish) and high (seawater-like) ionic strength by using 20 and 600 mM aqueous NaCl solutions. It is shown that MXene/activated-carbon asymmetric cell design capitalizes on the permselective behavior of MXene in sodium removal, which in turn forces carbon to mirror the same behavior in the removal of chloride ions. This has minimized the notorious co-ion desorption of carbon in highly saline media (600 mM NaCl) and boosted the charge efficiency from 4% in a symmetric activated-carbon/activated-carbon cell to 85% in a membrane-less asymmetric MXene/activated-carbon cell. Stable electrochemical performance for up to 100 cycles is demonstrated, yielding average desalination capacities of 8 and 12 mg/g, respectively, for membrane-less MXene/activated-carbon cells in NaCl solutions of 600 mM (seawater-level) and 20 mM (brackish-water-level). In the case of the 20 mM NaCl solutions, surprising charge efficiency values of over 100% have been obtained, which is attributed to the role of MXene interlayer surface charges.