In this study, a novel catalytic ceramic membrane (ITC-2-800@CM) was modified with Fe/N/S doped cyanobacterial biochar catalysts to adjust its surface morphology and properties to significantly enhance its organic pollutant removal performance and membrane anti-fouling ability. Specifically, the biochar modification further increased the roughness and hydrophobicity of the pristine ceramic membrane, apparently improving the adsorption capacity of hydroxychloroquine (HCQ) causing membrane fouling. Although sacrificing partial membrane permeability, based on the strong peroxymonosulfate (PMS) activation performance of cyanobacterial biochar, abundant reactive oxygen species were generated and degraded the organic pollutants adsorbed on the surface and pore of ITC-2-800@CM. Hence, the efficient synergistic effect between in situ adsorption, filtration and PMS activation further enhanced hydroxychloroquine removal and membrane anti-fouling performance, especially under a long operation. The actual lake water treatment experiments demonstrated that the ITC-2-800@CM–PMS system could stably remove more than 90% of HCQ and reduce the reversible and irreversible membrane fouling resistance by 81.57% and 60.68% as compared to the pristine CM/PMS system. Furthermore, the treated effluent showed significant reduction in total nitrogen, dissolved organic carbon and UV254 concentrations, highlighting the high applicability of the ITC-2-800@CM–PMS system in practical polluted water treatment. This improvement can decrease the need for frequent membrane cleaning during water treatment, thereby reducing operational costs. This research not only provided an easy method for ceramic membrane modification to extend its operational lifespan, but also offered deeper insights into the synergistic effect between in situ filtration and advanced oxidation.
Ferrate (Fe(VI), FeO 4 2- ) has been widely used in the degradation of micropollutants with the advantages of high redox potential , no secondary pollution and inhibition of disinfection byproducts . However, the low transformation of Fe(V) and/or Fe(IV) by Fe(VI) and incomplete mineralization of pollutants limit their application. In this work, we designed a photo electric cell with TiO 2 nanotubes (TNTs) and Pt serving as the anode and cathode to enhance the utilization of Fe(VI) (Fe(VI)-TNTs system). TNTs accelerated the generation of •OH via h VB + oxidation of OH - and photogenerated electrons at Pt boosted the transformation of Fe(VI) to Fe(V) and/or Fe(IV), resulting in a 22.2 % enhancement of chloroquine (CLQ) removal compared to Fe(VI) alone. The results from EPR and quenching tests showed that Fe(VI), Fe(V), Fe(IV), •OH, O 2 •- and h VB + coexisted in the Fe(VI)-TNTs system, among which Fe(V) and Fe(IV) were testified as the primary reactive substances accounting for 59 % of CLQ removal. The performance tests and recycling tests demonstrated that the Fe(VI)-TNTs system maintained excellent performance in an authentic water environment. The plausible degradation pathway of CLQ oxidized in the Fe(VI)-TNTs system was proposed with nine identified oxidation products via N-C cleavage, electrophilic addition and carboxylation processes. Based on the ECOSAR calculation, the constructed reaction system allowed a decrease in acute and chronic toxicity. Our findings provide a highly efficient and cost-effective strategy to enhance Fe(VI) application for micropollutant degradation in the future.
A photocathode-microbial electrochemical coupling system (PC-MFC) using black phosphorus-doped titanium dioxide nanobelt (BP/TB) as a photocatalyst is constructed for the degradation of hydroxychloroquine (HCQ, used to treat COVID-19). The degradation efficiency of HCQ (100 mg/L) in coupling system is 73.7% within 8 h, higher than that of photocatalysis (69.5%), MFC (25.6%), and adsorption (9.6%). The photocathode coupling facilitates subsequent bioelectric treatment, resulting in complete degradation of HCQ (100 mg/L) within 96 h in PC-MFC, much higher than in MFC (51.1%). Illumination of PC-MFC significantly increases the cathodic abundance of Pseudomonadales ord. (from 1.83% to 66.30%), accumulates biomass, improves the electrochemical behaviors of photocathode and bioanode , and finally increases the maximum power from 241 to 280 mW/m 2 . The electron transfer pathways depende on nicotinamide adenine dinucleotide dehydrogenase, succinate dehydrogenase and terminal oxidase. The coupled system enhances the dechlorination reduction of HCQ and reduces the biotoxicity of its degradation pathway . PC-MFC represents a new strategy for the treatment and energy recovery of refractory organic compounds in wastewater.
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