Fabrication of visible-light-responsive, macroscopic photo-Fenton catalysts is crucial for wastewater treatment. Here, we report a facile fabrication method for nano-FeO(OH)/reduced graphene oxide aerogels (FeO(OH)-rGA) equipped with a stable macrostructure and a high efficiency for catalytic degradation of phenolic organics. The structure of FeO(OH)/rGA was characterized by SEM, TEM, XPS, Raman analysis. The FeO(OH) is the main constituent of ferrihydrite, which dispersed in the graphene aerogel with a particle size of ∼3 nm can efficiently activate HO to generate abundant •OH. The excellent performance of the FeO(OH)/rGO aerogel was specifically exhibited by the outstanding catalyst activity, sustained mineralization and eminent reaction rate for phenolic organics. A synergy effect between FeO(OH) and graphene aerogel was observed, which came from the extensive electron transfer channels and active sites of the 3D graphene aerogel and the visible-light-activated FeO(OH) and HO consistently producing •OH. The FeO(OH)/rGA could be reused for 10 cycles without a reduction in the catalytic activity and had less iron leaching, which guarantees that the active ingredient remains in the gel. Moreover, the FeO(OH)/rGA induced photo-Fenton degradation of 4-chlorophenol under near neutral pH conditions because the tight connection of FeO(OH) with the rGO aerogel results in less iron leaching and prevents the generation of Fe(OH). The 4-chlorophenol was completely removed in 80 min with a 0.074 min rate constant in the FeO(OH)-rGA/HO photo-Fenton system under visible-light irradiation, and mineralization rate was up to 80% after 6 h. Oxidative •OH can continuously attack 4-chlorophenol, 2,4,6-trichlorophenol and bisphenol A without selectivity. These results lay a foundation for highly effective and durable photo-Fenton degradation of phenolic organics at near neutral pH and sufficient activation of HO for future applications.
Graphene oxide (GO) contains not only aromatic carbon lattice but also carboxyl groups which enhanced the aqueous solubility of GO. To study the transformation of GO nanosheets in natural environments, GO aqueous dispersion was mixed with Fe3+ ions to form photoactive complex. Under visible light irradiation, Fe(III) of the complex would be reduced to Fe(II) which could subsequently reduce highly toxic Cr(VI) to Cr3+. The electron of the reduction was contributed by the decarboxylation of carboxyl groups on GO and iron was acting as a catalyst during the photoreduction. On the other hand, the consumption of carboxyl groups may convert GO to rGO which are tend to aggregate since the decreased electrostatic repulsion and the increased π-π attraction. The formed Cr3+ may be electrostatically adsorbed by the rGO sheets and simultaneously precipitated with the aggregated rGO sheets, resulting the effective removal of chromium and GO nanosheets from the aqueous environment. This study may shed a light on understanding the environmental transformation of GO and guide the treatment of Cr(VI).
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