RESUMO
This study explores the use of silica-coated bacterial nanocellulose (BC) scaffolds with bulk macroscopic yet nanometric internal pores/structures as functional supports for high surface area titania aerogel photocatalysts to design flexible, self-standing, porous, and recyclable BC@SiO2-TiO2 hybrid organic-inorganic aerogel membranes for effective in-flow photo-assisted removal of organic pollutants. The hybrid aerogels were prepared by sequential sol-gel deposition of the SiO2 layer over BC, followed by coating of the resulting BC@SiO2 membranes with a porous titania aerogel overlayer of high surface area using epoxide-driven gelation, hydrothermal crystallization, and subsequent supercritical drying. The silica interlayer between the nanocellulose biopolymer scaffold and the titania photocatalyst was found to greatly influence the structure and composition, particularly the TiO2 loading, of the prepared hybrid aerogel membranes, allowing the development of photochemically stable aerogel materials with increased surface area/pore volume and higher photocatalytic activity. The optimized BC@SiO2-TiO2 hybrid aerogel showed up to 12 times faster in-flow photocatalytic removal of methylene blue dye from aqueous solution in comparison with bare BC/TiO2 aerogels and outperformed most of the supported-titania materials reported earlier. Moreover, the developed hybrid aerogels were successfully employed to remove sertraline drug, a model emergent contaminant, from aqueous solution, thus further demonstrating their potential for water purification.
Assuntos
Dióxido de Silício , Titânio , Dióxido de Silício/química , Titânio/química , Biopolímeros/química , Água/químicaRESUMO
The catalytic activity of layered double hydroxides, with and without insertion of copper, was evaluated in a heterogeneous Fenton process for degradation of the antibiotic sulfathiazole (STZ). The characterizations with different techniques revealed lamellar structures formed by stacking of layers containing magnesium, iron, and copper cations. The insertion of copper in the lamellar structure increased the specific area of the material and the degradation kinetics, achieving complete STZ removal after 90 min. X-ray photoelectron spectroscopy analysis showed the presence of Cu(II) and Cu(I) surface sites, which contributed to the generation of hydroxyl and hydroperoxyl/superoxide radicals. It also indicated an increase of Cu(I) content after use. For both materials, but specially for LDH without copper, addition of tert-butyl alcohol and p-benzoquinone hindered STZ degradation, indicating the importance of hydroxyl and hydroperoxyl/superoxide radicals in the degradation process, respectively. These results demonstrated the potential of copper-modified MgFe-CO3 as a catalyst for the degradation of emerging contaminants, offering the benefits of easy preparation and high efficiency in the Fenton process.
RESUMO
In this article, a light-emitting diode (LED)-based photoreactor was designed and evaluated for degradation of the antibiotic sulfathiazole (STZ), using heterogeneous photo-Fenton process with an iron ore residue as catalyst. The effects of the type of magnetic stirrer bar, use of baffles, rotation speed, and type and intensity of irradiation source were evaluated. The results showed that the degradation of STZ was strongly influenced by rotation speed (1100 rpm) and that the use of an octagonal stirrer bar favoured high dispersion and greater contact of the catalyst with the reaction medium. Although the presence of baffles had little influence on STZ degradation, their use enabled good dispersion of the catalyst (due to axial flow) and eliminated the vortex formed at high stirring speeds. It was found that the iron mining residue could be activated by UV LEDs, visible light LEDs, and black light irradiation, with similar degradation efficiencies achieved. Using the LEDs, STZ concentrations below the detection limit were obtained after 40 min, with power consumption 38-fold (UV LEDs) and 22-fold (visible light LEDs) lower than required for black light irradiation. The results demonstrated the advantages of the use of LED devices as irradiation systems in heterogeneous photo-Fenton processes.