Blend-electrospun graphene oxide/Poly(vinylidene fluoride) nanofibrous membranes with high flux, tetracycline removal and anti-fouling properties

Abstract

Graphene oxide (GO)/poly(vinylidene fluoride) (PVDF) electrospun nanofibrous membranes (ENMs) have been fabricated to remove tetracycline (TC) from water via adsorptive-filtration. The pure water permeation flux of GO/PVDF ENMs (27,407–29,337 LMH/bar) was increased compared with that of PVDF ENMs. The flow pore diameter was steadily reduced by increasing the GO content from 0 to 1.5 wt% in the GO/PVDF ENMs. The maximum TC adsorption capacity of GO is 720.26 mg/g (Langmuir model) and GO retained its TC adsorption property after incorporation into GO/PVDF ENMs during water filtration (transmembrane pressure = 0.91 bar). The maximum experimental TC removal capacity (qa,exp) was 17.92 mg/g with 1.5 wt% of GO (GO1.5/PVDF) ENMs, which was similar to the modified dose-response model value of 18.03 mg/g. In the presence of natural organic matter, TC adsorption was enhanced, because hydrophobic organic carbon improved hydrophobic and π-π interactions. The presence of Cu(II) further improved the TC adsorption capacity of GO1.5/PVDF ENMs through cation bridging. However, the presence of Ca(II) hindered TC adsorption by an electron shielding effect. For examining anti-fouling activity of GO1.5/PVDF ENMs, the log removal values of both bacteria, Escherichia coli and Staphylococcus aureus, were maintained at over 5 during water filtration. In addition, incorporation of GO in PVDF ENMs prevents bovine serum albumin (BSA) adsorption by both increasing the hydrophilicity of the ENMs forming hydration layer on the surface and electrostatic repulsion between both negatively charged BSA and GO in GO1.5/PVDF ENMs (zeta potential = - 14.14 mV, deionized water at pH 6).