Beetle‐Inspired Assembly of Heterostructured Lamellar Membranes with Polymer Cluster–Patterned Surface for Enhanced Molecular Permeation

Abstract 2D lamellar membranes hold great promise in efficient molecular separations of liquid and gas mixtures. However, the simultaneous realization of high permeation and precise sieving (i.e., overcoming the permeation–rejection tradeoff) of membranes poses a great challenge. Inspired by the structures and functions of the beetle's back, the heterostructured lamellar membranes fabricated through facile and controllable electrostatic atomization method are reported. Particularly, hydrophobic polymer clusters are patterned on hydrophilic laminate (graphene oxide) surfaces to realize the hydrophilic/hydrophobic heterostructure. It shows that the fast dissolution for nonpolar solvents is achieved by the strong affinity polymer clusters, and the ultralow‐barrier diffusion is achieved by the weak affinity laminate channels. Therefore, the permeance is remarkably enhanced (over 7 times for nonpolar solvents), while fully retaining membrane rejection. In contrast, hydrophilic clusters are patterned on hydrophobic laminate (reduced graphene oxide) surfaces and exhibit similar behaviors toward polar solvents. Furthermore, the lamellar membrane displays highly ordered layer‐by‐layer stacking, affording precise molecular rejection. Besides, the lamellar membrane acquires lower thermodynamic energy and hence superior stability under ultrasonic and strong acid or alkali environments, manifesting great potential for long‐term practical operation.