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Characterization and Computation of Yb/TiO? and Its Photocatalytic Degradation with Benzohydroxamic Acid.

ABSTRACT: Yb-doped TiO? (Yb/TiO?) compositions were synthesized by sol-gel method, and the prepared materials were characterized by X-ray Diffraction (XRD), X-ray photoelectron spectroscopy (XPS), UV-visible diffuse-reflectance spectrum (UV-Vis DRS), transmission electron microscope (TEM) and high resolution transmission electron microscope (HRTEM), energy dispersive spectrometer (EDS), and N? adsorption. A beneficiation reagent of benzohydroxamic acid (BHA) was used to test the photocatalytic activity of Yb/TiO?. The characterizations indicate that the doping of Yb could inhibit the crystal growth of TiO?, enhance the specific surface area, increase the binding energy of Ti2p, and also slightly expand the adsorption ranges to visible light. Furthermore, the computation of band structure also indicates that Yb-doped TiO? could make the forbidden band narrower than pure anatase TiO?, which presents a red shift in the absorption spectrum. As a result of the photodegradation experiment on BHA, Yb/TiO? (0.50% in mass) sintered at 450 °C displayed the highest catalytic activity for BHA when compared with pure TiO? or other doped Yb/TiO? compositions, and more than 89.2% of the total organic carbon was removed after 120 min. Almost all anions, including Cl-, HCO?-, NO?-, and SO?2-, inhibited the degradation of BHA by Yb/TiO?, and their inhibition effects followed the order of HCO?- > NO?- > SO?2- > Cl-. Cations of Na?, K?, Ca2+, and Mg2+ displayed a slight suppressing effect due to the impact of Cl- coexisting in the solution. In addition, Yb/TiO? maintained a high photocatalytic ability with respect to BHA after four runs. It is hypothesized that ·OH is one of the main species involved in the photodegradation of BHA, and the mutual transformation of Yb3+ and Yb2+ could promote the separation of electron-hole pairs.

SUBMITTER: Luo X

PROVIDER: S-EPMC5750890 | biostudies-other | 2017 Nov

REPOSITORIES: biostudies-other

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Characterization and Computation of Yb/TiO₂ and Its Photocatalytic Degradation with Benzohydroxamic Acid.

Luo Xianping X Zhu Sipin S Wang Junyu J Wang Chunying C Wu Min M

International journal of environmental research and public health 20171128 12

Yb-doped TiO₂ (Yb/TiO₂) compositions were synthesized by sol-gel method, and the prepared materials were characterized by X-ray Diffraction (XRD), X-ray photoelectron spectroscopy (XPS), UV-visible diffuse-reflectance spectrum (UV-Vis DRS), transmission electron microscope (TEM) and high resolution transmission electron microscope (HRTEM), energy dispersive spectrometer (EDS), and N₂ adsorption. A beneficiation reagent of benzohydroxamic acid (BHA) was used to test the photocatalytic activity of ...[more]

PMID: 29182555

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Project description:Perfluorooctanoic acid (PFOA), a typical perfluorinated carboxylic acid, is an emerging type of permanent organic pollutants that are regulated by the Stockholm Convention. The degradation of PFOA, however, is quite challenging largely due to the ultra-high stability of C-F bonds. Compared with other techniques, photocatalytic degradation offers the potential advantages of simple operation under mild conditions as well as exceptional decomposition and defluorination efficiency. Titanium dioxide (TiO2) is one of the most frequently used photocatalysts, but so far, the pristine nanosized TiO2 (e.g., the commercial P25) has been considered inefficient for PFOA degradation, since the photo-generated hydroxyl radicals from TiO2 are not able to directly attack C-F bonds. Mesoporous Sb2O3/TiO2 heterojunctions were therefore rationally designed in this work, of which the confined Sb2O3 nanoparticles in mesoporous TiO2 framework could not only tune the band structure and also increase the number of active sites for PFOA degradation. It was found that, after loading Sb2O3, the absorption of UV light was enhanced, indicating a higher efficiency of light utilization; while the band gap was reduced, which accelerated the separation of photo-generated charge carriers; and most importantly, the valence band edge of the Sb2O3/TiO2 heterojunction was significantly lifted so as to prevent the occurrence of hydroxyl radical pathway. Under the optimal ratio of Sb2O3-TiO2, the resulting catalysts managed to remove 81.7% PFOA in 2 h, with a degradation kinetics 4.2 times faster than the commercial P25. Scavenger tests and electron spin resonance spectra further revealed that such improvement was mainly attributed to the formation of superoxide radicals and photo-generated holes, in which the former drove the decarboxylation from C7F15COOH-C7F15 •, and the latter promoted the direct electron transfer for the conversion of C7F15COO--C7F15COO•. The Sb2O3/TiO2 photocatalysts were highly recyclable, with nearly 90% of the initial activity being retained after five consecutive cycles, guaranteeing the feasibility of long-term operation.

Dataset Information

Characterization and Computation of Yb/TiO? and Its Photocatalytic Degradation with Benzohydroxamic Acid.

Publications

Characterization and Computation of Yb/TiO₂ and Its Photocatalytic Degradation with Benzohydroxamic Acid.

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