Electroactive membrane with the electroactive layer beneath the separation layer to eliminate the interference of humic acid in the oxidation of antibiotics

Removing harmful antibiotics is essential to reclaiming water from municipal secondary effluent. Electroactive membranes are effective in the removal of antibiotics but challenged by the abundant coexisting macromolecular organic pollutants in municipal secondary effluent. To eliminate the interference of macromolecular organic pollutants in the removal of antibiotics, we propose a novel electroactive membrane with a top polyacrylonitrile (PAN) ultrafiltration layer and a bottom electroactive layer composed of carbon nanotubes (CNTs) and polyaniline (PANi). When filtering the mixture of tetracycline (TC, a typical antibiotic) and humic acid (HA, a typical macromolecular organic pollutant), the PAN-CNT/PANi membrane performed sequential removal. It retained HA at the PAN layer (by ∼96%) and allowed TC to reach the electroactive layer where it was electrochemically oxidized (e.g., by ∼92% at 1.5 V). The TC removal of the PAN-CNT/PANi membrane was marginally affected by HA, unlike that of the control membrane with the electroactive layer on the top that showed decreased TC removal after the addition of HA (e.g., decreased by 13.2% at 1 V). The decreased TC removal of the control membrane was attributed to the attachment (but not competitive oxidation) of HA on the electroactive layer that impaired the electrochemical reactivity. The HA removal prior to TC degradation realized by the PAN-CNT/PANi membrane avoided the attachment of HA and guaranteed TC removal on the electroactive layer. Long-term filtration for 9 h revealed the stability of the PAN-CNT/PANi membrane, and its advantageous structural design was conformed in the context of real secondary effluents.