Stress driven micron- and nano-scale wrinkles as a new class of transport pathways of two-dimensional laminar membranes towards molecular separation

Narrow and tortuous interstitial paths through parallelly oriented interlayer spacings hinder the practical viability of 2D laminar membranes due to the limited membrane permeance. Ubiquitous stress involved wrinkling morphologies of biological tissues inspire us to exploit spontaneously formed wrinkles for facilitating transmembrane molecular transport. Herein, a stress driven wrinkle engineering methodology is proposed for manipulating micron- and nano-scale wrinkles as a new class of transport pathways of GO membranes. Micron-scale wrinkles of GO laminates are initiated by capillary stress via good solvents evaporation, while nano-scale wrinkles of GO nanosheets are induced by entropy stress via poor solvents resolvation. The deliberately tailored GO membranes possess nanoarchitectures with both high porous volume and low defective degree, thus achieving remarkable molecular separation performances (water permeance of ∼69.2 L m−2 h−1 bar−1and dye rejection of >98%). This work offers a straightforward experimental strategy for designing high-performance 2D laminar membranes via rational wrinkle manipulations.