Organic Fouling of Graphene Oxide Membranes and Its Implications for Membrane Fouling Control in Engineered Osmosis

This study provides experimental evidence to mechanistically understand some contradicting effects of the characteristic properties of graphene oxide (GO), such as the high hydrophilicity, negative charge, strong adsorption capability, and large surface area, on the antifouling properties of GO membranes. Furthermore, this study demonstrates the effectiveness of forming a dense GO barrier layer on the back (i.e., porous) side of an asymmetric membrane for fouling control in pressure-retarded osmosis (PRO), an emerging engineered osmosis process whose advancement has been much hindered due to the severe irreversible fouling that occurs as foulants accumulate inside the porous membrane support. In the membrane fouling experiments, protein and alginate were used as model organic foulants. When operated in forward osmosis mode, the GO membrane exhibited fouling performance comparable with that of a polyamide (PA) membrane. Analysis of the membrane adsorption capacity showed that, likely due to the presence of hydrophobic regions in the GO basal plane, the GO membrane has an affinity toward organic foulants 4 to 5 times higher than the PA membrane. Such a high adsorption capacity along with a large surface area, however, did not noticeably aggravate the fouling problem. Our explanation for this phenomenon is that organic foulants are adsorbed mainly on the basal plane of GO nanosheets, and water enters the GO membrane primarily around the oxidized edges of GO, making foulant adsorption not create much hindrance to water flux. When operated in PRO mode, the GO membrane exhibited much better antifouling performance than the PA membrane. This is because unlike the PA membrane for which foulants can be easily trapped inside the porous support and hence cause severe irreversible fouling, the GO membrane allows the foulants to accumulate primarily on its surface due to the sealing effect of the GO layer assembled on the porous side of the asymmetric membrane support. Results from the physical cleaning experiments further showed that the water flux of GO membranes operated in PRO mode can be sufficiently restored toward its initial prefouling level.