Facilitated water transport in composite reduced graphene oxide pervaporation membranes for ethanol upgrading

Abstract

High purity ethanol is one of the most sought-after renewable energy sources. However, standard production methods yield ethanol of insufficient quality. Membrane processes such as pervaporation are recognized as a viable method for upgrading ethanol. Their performance and selectivity depend solely on membrane employed. Hydrophilic polyvinyl alcohol (PVA) membranes are used industrially for this purpose, but there is a trade-off between selectivity and permeability. Among other materials, chemically converted graphene attracts particular attention due to its exceptional water transport properties, however its application is limited by the fabrication of free-standing membranes. In this study, a composite reduced PVA/graphene oxide (rGO) membranes with different rGO content (up to 49 wt%) was synthesized. Polyvinyl alcohol acted as a mediator to improve the mechanical stability of membrane layers by crosslinking rGO flakes with hydrogen bonds. The resulting membranes were fully characterized by scanning electron microscopy, X-ray diffraction, Fourier-transform infrared spectroscopy, water contact angle and mechanical tests. Pervaporation tests with water/ethanol mixtures (10/90 wt%) at temperatures between 20 and 50 °C demonstrated an excellent selectivity (over 12000) of membranes and satisfactory flux, even at high temperatures. The total permeate flux for membranes varied slightly as a function of operating temperature, demonstrating a good thermostability of the reduced graphene oxide-based membranes. The pervaporation separation index (PSI) of synthesized membrane exceed 5000 and surpassed majority of rGO containing membranes reported in the literature. Results indicate that rGO membranes noncovalently strengthened with PVA are a promising material for selective ethanol dehydration via pervaporation.