Nanowire-assisted electrochemical perforation of graphene oxide nanosheets for molecular separation

Abstract

Two-dimensional nanosheets, e.g., graphene oxide (GO), have been widely used to fabricate efficient membranes for molecular separation. However, because of poor transport across nanosheets and high width-to-thickness ratio, the permeation pathway length and tortuosity of these membranes are extremely large, which limit their separation performance. Here we report a facile, scalable, and controllable nanowire electrochemical concept for perforating and modifying nanosheets to shorten permeation pathway and adjust transport property. It is found that confinement effects with locally enhanced charge density, electric field, and hydroxyl radical generation over nanowire tips on anode can be executed under low voltage, thereby inducing confined direct electron loss and indirect oxidation to reform configuration and composition of GO nanosheets. We demonstrate that the porous GO nanosheets with a lot of holes are suitable for assembling separation membranes with tuned accessibility, tortuosity, interlayer space, electronegativity, and hydrophilicity. For molecular separation, the prepared membranes exhibit quadruple water permeance and higher rejections for salts (>91%) and small molecules (>96%) as/than original ones. This nanowire electrochemical perforation concept offers a feasible strategy to reconstruct two-dimensional materials and tune their transport property for separation.