Degradation of aqueous 2,4,4'-Trihydroxybenzophenone by persulfate activated with nitrogen doped carbonaceous materials and the formation of dimer products.
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abstract
In this work, we systematically investigated the persulfate (PS) activation potential of a series of nitrogen doped carbonaceous materials for the degradation of 2,4,4'-trihydroxybenzophenone (2,4,4'-HBP), an additive in polyvinyl acetate films and personal care products. Nitrogen originating from urea, NH4NO3, indole and polyaniline was doped into carbonaceous materials, including hydroxylated multi-walled carbon nanotubes (CNT-OH), large-inner thin-walled carboxylated carbon nanotubes (CNT-COOH) and graphite oxide (GO), to examine the catalytic effect. The NH4NO3-CNT-OH catalyst, which showed the best catalytic performance in 2,4,4'-HBP removal, was characterized by SEM, TEM, FT-IR, Raman, BET surface area, XRD and XPS, and pyrrolic nitrogen was found to play a highly important role in the activation of PS. Under the conditions of [2,4,4'-HBP]0: [PS]0=1: 500, T=25C, pH0=7.0, concentration of catalyst=100mgL-1, 43.48M 2,4,4'-HBP was completely removed in 2h. According to electron paramagnetic resonance (EPR) spectra and radical quenching experiments, hydroxyl and sulfate radicals on the surface of the catalyst contributed to the substrate oxidation. Cleavage of C-C bridge bond, hydroxylation and polymerization were mainly involved in the oxidation process, leading to the formation of 10 intermediates (e.g., dimers), as detected by the MS/MS spectra. To the best of our knowledge, this report is the first to describe the transformation mechanism of 2,4,4'-HBP in nitrogen doped carbonaceous materials catalyzed PS system.
