Co-based peroxymonosulfate (PMS) activation system with fascinating catalytic performance has become a promising technology for water purification, but it always suffers from insufficient mass transfer, less exposed active sites and toxic metal leaching. In this work, a carbon nanotube membrane confining Co3O4 inside (Co3O4-in-CNT) was prepared and was coupled with PMS activation (catalytic membrane process) for sulfamethoxazole (SMX) removal. Compared with counterpart with surface-loaded Co3O4 (Co3O4-out-CNT), the Co3O4-in-CNT catalytic membrane process exhibited enhanced SMX removal (99.5% vs. 89.1%) within residence time of 2.89 s, reduced Co leaching (20 vs. 147 μg L-1) and more interestingly, the nonradical-to-radical mechanism transformation (from 1O2 and electron transfer to SO4•- and •OH). These phenomena were ascribed to the nanoconfinement effect in CNT, which enhanced mass transfer (2.80 × 10-4 vs. 5.98 × 10-5 m s-1), accelerated Co3+/Co2+ cycling (73.4% vs. 65.0%) and showed higher adsorption energy for PMS (cleavage of O-O bond). Finally, based on the generated abundant reactive oxygen species (ROS), the seven degradation pathways of SMX were formed in system.
Keywords: Carbon nanotube membrane; Nanoconfinement effect; Peroxymonosulfate activation; Sulfamethoxazole removal; Theoretical calculation.
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