Free-standing graphene oxide thin films assembled by a pressurized ultrafiltration method for dehydration of ethanol

Free-standing graphene oxide (GO) thin films have been assembled by a pressurized ultrafiltration method. The GO films exhibit a layered microstructure with high structural stability and hydrophilicity, as analyzed by XPS, FESEM, XRD, positron annihilation spectroscopy (PAS), etc. The effects of ultrafiltration pressure and feed composition on the film׳s microstructure and pervaporation performance for dehydration of ethanol were investigated and correlated with XRD and PAS observations. Experimental results suggest that the interlaminar spacing is determined by both packing density of GO nanosheets and water content in the feed solution. The packing density is sensitively affected by the ultrafiltration pressure applied during film formation. By tuning the ultrafiltration pressure, a high separation performance with water permeability of 13,800Barrer (1 Barrer=3.348×10−19 kmol m m−2 s−1 Pa−1) and water/ethanol selectivity of 227 is achieved for dehydration of an 85wt% ethanol aqueous solution at 24°C. Additionally, the total permeability varied from 50 to 113,000Barrer by increasing the water content in the feed from 0 to 100wt%. As a result, the ideal water/ethanol selectivity calculated from single-component feed tests is about 2260 which is much higher than the selectivity obtained from binary-component feed tests. This discrepancy is probably attributed to the effect of intermolecular hydrogen bonding between water molecules and the functional groups on GO nanosheets that enlarges the interlaminar spacing and allows more ethanol transport through the GO film. The interactions among the GO nanosheets and the feed components enable the film to effectively dehydrate ethanol via pervaporation. [Display omitted] •A facile ultrafiltration method is developed to assemble the GO films.•The films exhibit a well-packed microstructure with high structural stability.•The interlaminar spacing is sensitive to both ultrafiltration pressure and feed composition.•The GO films show particularly high water permeability as well as outstanding selectivity.