Elucidating Ultrafast Molecular Permeation through Well-Defined 2D Nanochannels of Lamellar Membranes

Angew Chem Int Ed Engl. 2019 Dec 16;58(51):18524-18529. doi: 10.1002/anie.201912570. Epub 2019 Nov 6.

Abstract

Lamellar membranes with well-defined 2D nanochannels show fast, selective permeation, but the underlying molecular transport mechanism is unexplored. Now, regular robust MXene Ti3 C2 Tx lamellar membranes are prepared, and the size and wettability of nanochannels are manipulated by chemically grafted hydrophilic (-NH2 ) or hydrophobic (-C6 H5 , -C12 H25 ) groups. These nanochannels have a sharp difference in mass transfer behavior. Hydrophilic nanochannels, in which polar molecules form orderly aligned aggregates along channel walls, impart ultrahigh permeance (>3000 L m-2 h-1 bar-1 ), which is more than three times higher than that in hydrophobic nanochannels with disordered molecular configuration. In contrast, nonpolar molecules with disordered configuration in both hydrophilic and hydrophobic nanochannels have comparable permeance. Two phenomenological transport models correlate the permeance with the mass transport mechanism of molecules that display ordered and disordered configuration.

Keywords: MXene Ti3C2Tx nanosheet; lamellar membranes; molecular alignment; molecular transport mechanism; ultrafast solvent permeation.