A New Strategy for Highly Efficient Separation between Monovalent Cations by Applying Opposite-Oriented Pressure and Electric Fields.

Biological ion channels exhibit excellent ion selectivity, but it has been challenging to design their artificial counterparts, especially for highly efficient separation of similar ions. Here, a new strategy to achieve high selectivity between alkali metal ions with artificial nanostructures is reported. Molecular dynamics (MD) simulations and experiments are combined to study the transportation of monovalent cations through graphene oxide (GO) nanoslits by applying pressure or/and electric fields. It is found that the ionic transport selectivity under the pressure driving reverses compared with that under the electric field driving. Moreover, MD simulations show that different monovalent cations can be separated with unprecedentedly high selectivity by applying opposite-oriented pressure and electric fields. This highly efficient separation originates from two distinctive ionic transporting modes, that is, hydration shells drive ions under pressure, but drag ions under the electric field. Hence, ions with different hydration strengths can be efficiently separated by tuning the net mobility induced by the two types of driving forces when the selected ions are kept moving while the other ones are immobilized. And nanoconfinement is confirmed to enhance the separation efficacy. This discovery paves a new avenue for separating similar ions without elaborately designing biomimetic nanostructures.

The Selective Transport of Ions in Charged Nanopore with Combined Multi-Physics Fields.

The selective transport of ions in nanopores attracts broad interest due to their potential applications in chemical separation, ion filtration, seawater desalination, and energy conversion. The ion selectivity based on the ion dehydration and steric hindrance is still limited by the very similar diameter between different hydrated ions. The selectivity can only separate specific ion species, lacking a general separation effect. Herein, we report the highly ionic selective transport in charged nanopore through the combination of hydraulic pressure and electric field. Based on the coupled Poisson-Nernst-Planck (PNP) and Navier-Stokes (NS) equations, the calculation results suggest that the coupling of hydraulic pressure and electric field can significantly enhance the ion selectivity compared to the results under the single driven force of hydraulic pressure or electric field. Different from the material-property-based ion selective transport, this method endows the general separation effect between different kinds of ions. Through the appropriate combination of hydraulic pressure and electric field, an extremely high selectivity ratio can be achieved. Further in-depth analysis reveals the influence of nanopore diameter, surface charge density and ionic strength on the selectivity ratio. These findings provide a potential route for high-performance ionic selective transport and separation in nanofluidic systems.

Vertically-Oriented Ti3C2Tx MXene Membranes for High Performance of Electrokinetic Energy Conversion.

The electrokinetic effect to convert the mechanical energy from ambient has gained sustained research attention because it is free of moving parts and easy to be miniaturized for microscale applications. The practical application is constrained by the limited electrokinetic energy conversion performance. Herein, we report vertically oriented MXene membranes (VMMs) with ultrafast permeation as well as high ion selectivity, in which the permeation is several thousand higher than the largely researched horizontally stacked MXene membranes (HMMs). The VMMs can achieve a high streaming current of 8.17 A m-2 driven by the hydraulic pressure, largely outperforming all existing materials. The theoretical analysis and numerical calculation reveal the underlying mechanism of the ultrafast transport in VMMs originates from the evident short migration paths, the low energy loss during the ionic migration, and the large effective inlet area on the membrane surface. The orientation of the 2D lamella in membranes, the long-overlooked element in the existing literatures, is identified to be an essential determinant in the performance of 2D porous membranes. These understandings can largely promote the development of electrokinetic energy conversion devices and bring advanced design strategy for high-performance 2D materials.

Vertically Transported Graphene Oxide for High-Performance Osmotic Energy Conversion.

Reverse electrodialysis is a promising method to harvest the osmotic energy stored between seawater and freshwater, but it has been a long-standing challenge to fabricate permselective membranes with the power density surpassing the industry benchmark of 5.0 W m-2 for half a century. Herein, a vertically transported graphene oxide (V-GO) with the combination of high ion selectivity and ultrafast ion permeation is reported, whose permeation is three orders of magnitude higher than the extensively studied horizontally transported GO (H-GO). By mixing artificial seawater and river water, an unprecedented high output power density of 10.6 W m-2 is obtained, outperforming all existing materials. Molecular dynamics (MD) simulations reveal the mechanism of the ultrafast transport in V-GO results from the quick entering of ions and the large accessible area as well as the apparent short diffusion paths in V-GO. These results will facilitate the practical application of osmotic energy and bring an innovative design strategy for various systems involving ultrafast transport, such as filtration and catalysis.