Structurally Stable, Antifouling, and Easily Renewable Reduced Graphene Oxide Membrane with a Carbon Nanotube Protective Layer

The excellent permeability and selectivity of reduced graphene oxide (rGO) membranes have been demonstrated both theoretically and experimentally; however, strategies for the fabrication of highly stable, antifouling rGO membranes with facile recovery after fouling have rarely been investigated. In this work, we report a structurally durable rGO-based hollow fiber membrane that allows high-pressure (at least 1 bar) back-flushing. This is achieved by sandwiching the rGO layer between a carbon nanotube (CNT) protective layer and a polyacrylonitrile (PAN) support. The CNT layer could also function as a prefiltration and pre-adsorption microsystem and endow a higher resistance against fouling. This is experimentally confirmed by the much higher normalized permeance (0.82-0.92) of the CNT/rGO/PAN membranes than the simple rGO/PAN membranes (0.42-0.53) under the same operating conditions. Additionally, under a low cathode potential (0.9 V), the membrane could easily be renewed after fouling by simple back-flushing with a flux recovery ratio of similar to 96%. An investigation of the mechanism indicates that electrostatic repulsive forces promote the desorption of charged organic foulants (e.g., humic acid and dyes) from the rGO and CNT layers, and they can subsequently be removed from the membrane with water.