In this study, we fabricated carbonaceous composite membranes by loading integrated mats of nitrogen-doped graphene, reduced graphene oxide, and carbon nanotubes (NG/rGO/CNTs) on a nylon microfiltration substrate and employed it for in-situ catalytic oxidation by activating peroxydisulfate (PDS) for the removal of sulfamethoxazole (SMX) in a real water matrix. The impact of coexisting organics on the performance of carbonaceous catalysis was investigated in the continuous filtration mode. Reusability testing and radical quenching experiments revealed that the non-radical pathways of surface-activated persulfate mainly contributed to SMX degradation. A stable SMX removal flux (rSMX) of 22.15 mg m-2·h-1 was obtained in 24 h when tap water was filtered continuously under a low pressure of 1.78 bar and in a short contact time of 1.4 s, which was slightly lower than the rSMX of 23.03 mg m-2·h-1 performed with deionized water as the control group. In addition, higher contents of protein-, fulvic acid-, and humic acid-like organics resulted in membrane fouling and significantly suppressed SMX removal during long-term filtration. Changes in the production of sulfate ions and the Raman spectra of carbon mats indicated that organics prevent the structural defects of the carbon matrix from participating in PDS activation. Moreover, NG/rGO/CNTs composite membranes coupled with activated persulfate oxidation exhibited good self-cleaning ability, because membrane fouling could be partly reversed by restoring filtration pressure during operation. This study provides a novel and effective oxidation strategy for efficient SMX removal in water purification, allowing the application of carbonaceous catalysis for the selective degradation of emerging contaminants.
Keywords: Carbonaceous composite membranes; In-situ catalytic oxidation; Non-radical pathway; Peroxydisulfate activation; Real water matrix; Sulfamethoxazole.
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