Comediation of voltage gating and ion charge in MXene membrane for controllable and selective monovalent cation separation

Artificial ion channels with controllable mono/monovalent cation separation fulfill important roles in biomedicine, ion separation, and energy conversion. However, it remains a daunting challenge to develop an artificial ion channel similar to biological ion channels due to ion-ion competitive transport and lack of ion-gating ability of channels. Here, we report a conductive MXene membrane with polydopamine-confined angstrom-scale channels and propose a voltage gating and ion charge comediation strategy to concurrently achieve gated and selective mono/monovalent cation separation. The membrane shows a highly switchable "on-off" ratio of ∼9.9 for K⁺ transport and an excellent K⁺/Li⁺ selectivity of 40.9, outperforming the ion selectivity of reported membranes with electrical gating (typically 1.5 to 6). Theoretical simulations reveal that the introduced high-charge cations such as Mg²⁺ enable the preferential distribution of target K⁺ over competing Li⁺ at the channel entrance, and the surface potential reduces the ionic transport energy barrier for allowing K⁺ to pass quickly through the channel.