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1.
Dalton Trans ; 47(38): 13608-13615, 2018 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-30207359

RESUMO

Coupled adsorption and photocatalytic oxidation brings high expectations regarding the fast and efficient removal of gaseous pollutants in air. However, to fabricate an adsorbent-photocatalyst composite, coating of a photocatalyst on adsorbent support inevitably results in loss of adsorption and light blocking on interior surfaces. In this work, we attempt to develop an adsorbent-photocatalyst monolith composite, which not only perfectly retains original high adsorption capacity, but also allows complete penetration of UV light through the whole monolith. We employ a SiO2 aerogel monolith with a diameter of 2.5 cm and thickness of 0.7 cm as adsorbent and support. After atomic layer deposition (ALD) followed by calcination, 0.32-1.25 wt% TiO2 is dispersed on the skeleton of the SiO2 aerogel. In spite of such a low level of loading, the monolith composites exhibit fast and efficient removal of gaseous acetaldehyde and NO. Therein, the best performance is achieved at a loading of 0.6 wt% TiO2. By dark adsorption, the acetaldehyde pollutant with initial concentration of 200 ppm can be adsorbed by 54% within 10 min. Moreover, the light transmittance at 387 nm can be retained as high as 6% after penetrating through the whole monolith, confirming that all loaded TiO2 nanoparticles can participate in the photocatalytic oxidation of acetaldehyde. Under UV irradiation with intensity close to natural sunlight, the preadsorbed acetaldehyde can be completely mineralized into CO2 by photocatalytic oxidation in another 60 min, benefiting from the ultradispersion of TiO2 nanoparticles inside the SiO2 aerogel. The study provides a novel three-dimensional model of an adsorbent-photocatalyst composite for the fast and efficient removal of gaseous pollutants.

2.
Dalton Trans ; 46(44): 15363-15372, 2017 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-29072735

RESUMO

Doping and tailoring of the crystal orientation are two main strategies to improve the photocatalytic properties of TiO2 films. Herein, we introduce a novel route for obtaining Nb-doped TiO2 anatase films with the [001] preferred orientation by thermal oxidation of the [100]-oriented Nb-doped TiN film prepared by magnetron sputtering. Comprehensive analyses with X-ray diffraction, Raman scattering, high-resolution transmission electron microscopy, and X-ray photoelectron spectroscopy indicate that the proportion of high-energy (001) facets of the Nb-doped TiO2 film is more than 90% and the Nb5+ ion is successfully doped into the film without destroying the crystallinity and orientation. Moreover, the Nb5+ ion doping significantly restrains the growth of the TiO2 grains and increases the surface roughness, and consequently increases the surface-reactive sites. Therefore, the as-fabricated Nb-doped TiO2 film exhibits efficient photocatalytic oxidation performance for acetaldehyde and oleic acid decomposition under simulated solar light irradiation. Such Nb-doped TiO2 anatase films with high-reactivity (001) facet exposure may find applications in the photocatalysis and solar energy conversion fields.

3.
Dalton Trans ; 46(5): 1487-1494, 2017 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-28091650

RESUMO

The Schottky-type metal-semiconductor (M-S) junction works well in promoting the separation of photogenerated carriers. In this paper, another type of M-S junction, Ohmic contact of W@WO3, has been developed via an acid partial oxidation strategy. By simply tuning the experimental parameters including the acid concentration and the reaction time, WO3 nanosheets are epitaxially grown on a W core; moreover, the thickness and density of the WO3 shell can be finely controlled. The photocatalytic activities of samples are tested via degradation of gaseous acetaldehyde under UV light irradiation. The results show that the W@WO3 core-shell composite with a thinner and looser WO3 shell exhibits a higher mineralization ability of acetaldehyde to carbon dioxide. An Ohmic contact between the W core and the WO3 shell is fairly confirmed by means of photo-electronic measurements. It is believed that the built-in electric field at the interface of the Ohmic contact leads to the migration of photogenerated electrons from WO3 to W, which is beneficial for separation of the electron-hole pairs and hence an enhanced photooxidation ability.

4.
ACS Appl Mater Interfaces ; 7(14): 7752-8, 2015 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-25798532

RESUMO

Doping with impurities as well as introducing oxygen vacancies has been recognized as an important means to enhance photocatalytic activity of TiO2 under visible-light irradiation. Here we report that simple ethanol impregnation followed with mild heat treatment (150-400 °C) can color TiO2 nanoparticles and enhance visible-light photocatalytic activity of the material. The coloration and photocatalytic activity for ß-naphthol and rhodamine B (RhB) degradation were observed to be dependent on heat-treatment temperature, and the highest activity as well as the most coloration was obtained at temperatures around 200 to 250 °C. Comprehensive analyses based on X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) investigations as well as first-principle density functional calculation suggest that the simple ethanol impregnation treatment leads to the generation of oxygen vacancy on TiO2 surface which should be responsible for the coloration and enhanced photocatalytic activity.

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