RESUMEN
In order to study their synergistic catalytic effects in toluene degradation, CuMn2O4/HTS-1 (HTS-1 was a titanium silicon molecular sieve), Cu0.7Mn2Y0.3Ox/HTS-1 and Cu0.7Mn2Ce0.3Ox/HTS-1 catalysts were prepared by the impregnation method. The textural properties, redox properties and acidity of the catalysts were characterized by X-ray diffractometer (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), H2 temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), frustrated total internal reflection (FT-IR), ammonium temperature-programmed desorption (NH3-TPD) and pyridine adsorption internal reflection (Py-IR) measurements. The potential roles of Lewis acid sites (activating dioxygen) were discussed, and the experimental results indicated that the most efficient route for toluene degradation over Cu0.7Mn2Ce0.3Ox/HTS-1 (toluene conversion rate of 90% (T99)=295°C) was ascribed to regulation of the synergistic effects of redox properties (activating molecular toluene) and Lewis acid sites (activating dioxygen). The Mars-Van-Krevelen (MVK) model was adopted to describe the reaction process of toluene oxidation, which gave an in-depth view into the toluene degradation over CuMn2O4/HTS-1, Cu0.7Mn2Y0.3Ox/HTS-1 and Cu0.7Mn2Ce0.3Ox/HTS-1. In addition, the synergistic effects between redox properties and Lewis acid sites were studied in detail.
Asunto(s)
Modelos Químicos , Tolueno/química , Catálisis , Cobre/química , Manganeso/química , Oxidación-Reducción , Espectroscopía Infrarroja por Transformada de Fourier , TitanioRESUMEN
Herein, a non-stacked γ-Fe2O3/C@TiO2 double-layer hollow nano photocatalyst has been developed with ultrathin nanosheets-assembled double shells for photodegradation phenol. High catalytic performance was found that the phenol could be completely degraded in 135 min under visible light, due to the moderate band edge position (VB at 0.59 eV and CB at -0.66 eV) of the non-stacked γ-Fe2O3/C@TiO2, which can expand the excitation wavelength range into the visible light region and produce a high concentration of free radicals (such as ·OH, ·O2-, holes). Furthermore, the interior of the hollow composite γ-Fe2O3 is responsible for charge generation, and the carbon matrix facilitates charge transfer to the external TiO2 shell. This overlap improved the selection/utilization efficiency, while the unique non-stacked double-layered structure inhibited initial charge recombination over the photocatalysts. This work provides new approaches for photocatalytic applications with γ-Fe2O3/C-based materials.
RESUMEN
The mineralization of organic pollutants under visible light is challenging, limiting the practical application of photocatalytic technology in wastewater treatment. To achieve the efficient mineralization of Acid red 3R (AR3R), a series of honeycombed catalysts (TiO2, C-TiO2-X, Au@TiO2 and Au@C-TiO2-X) were prepared via a facile in situ synthetic method and characterized by XRD, TEM, BET, XPS and DRS, respectively. The introduction of C and Au species promote the simultaneous generation of â¢O2- and â¢OH over Au@C-TiO2-X under visible light radiation. The Au@C-TiO2-X catalyst showed superior performance for the deep mineralization of AR3R, affording a TOC removal rate larger than 90 % within 240â¯min under visible light (> 420â¯nm). The photocatalytic degradation mechanism of AR3R is proposed according to UV-vis and in situ DRIFTS analysis. The superior photocatalytic activity of Au@C-TiO2-X is attributed to the synergistic effect of â¢O2- and â¢OH owing to C doping and Au deposition.
RESUMEN
To achieve efficient degradation of toluene, a series of Cu1-yMn2CeyOx/sepiolite catalysts (yâ¯=â¯0.1, 0.2, and 0.3) with different Cu1-yMn2CeyOx loadings (10%, 20%, and 30%) were prepared via the co-precipitation method. The structure-activity and surficial elemental species of Cu1-yMn2CeyOx/sepiolite were characterized by XRD, TEM, SEM, BET, ICP-MS and XPS. The catalytic activity of the catalysts was tested in the oxidation reaction of toluene, results showed that 20%Cu0.8Mn2Ce0.2Ox/sepiolite remains able to remove toluene completely with high efficiency at a temperature of 289⯰C. Two kinetic models have been selected and tested to describe the oxidation of toluene, the Mars-van krevele (MVK) model provided a good fit (R2â¯≥â¯0.99). And the optimal relation of the surface oxidation activation energy (26.074â¯kJâ¯mol-1) and surface reduction activation energy (23.591â¯kJâ¯mol-1) were calculated.