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1.
Dye wastewater is a major source of toxic aromatic amines released into the environment. Semiconductor photocatalysis is a clean, solar-driven process for the treatment of dye wastewater. To enhance applicability of semiconductor photocatalysis, the catalyst used should be visible light active. Here we report a facile synthesis of a highly visible-light-active nitrogen-doped tungsten oxide, N-WO3, by thermal decomposition of peroxotungstic acid–urea complex. The structure and properties of N-WO3 are characterized by X-ray photoelectron spectroscopy and X-ray absorption near-edge spectroscopy. The photodegradation of amaranth catalyzed by N-WO3 is evaluated in a batch system under visible and ultraviolet A (UVA) light. Our results show successful doping of N in both interstitial and substitutional sites and the presence of N2-like species. The N doping surprisingly expands the usable portion of the solar spectrum up to the near-infrared region and enhances the photocatalytic activity. At typical experimental conditions such as 25 mg/L of amaranth, 1 g/L of N-WO3, and pH 7, 100 % degradation of amaranth is achieved within 2 h under both visible and UVA light. The photocatalytic activity of N-WO3 is maintained in repeated cycles, indicating its exceptional photostability. To the best of our knowledge, this is the first time that a reusable, highly visible-light-active N-WO3 can be obtained through thermal decomposition of peroxotungstic acid–urea complex.  相似文献   

2.
A solution of atrazine in a TiO2 suspension, an endocrine disruptor in natural water, was tentatively treated by microwave-assisted photocatalytic technique. The effects of mannitol, oxygen, humic acid, and hydrogen dioxide on the photodegradation rate were explored. The results could be deduced as follows: the photocatalytic degradation of atrazine fits the pseudo-first-order kinetic well with k = 0.0328 s?1, and ·OH was identified as the dominant reactant. Photodegradation of atrazine was hindered in the presence of humic acid, and the retardation effect increased as the concentration of humic acid increased. H2O2 displayed a significant negative influence on atrazine photocatalysis efficiency. Based on intermediates identified with gas chromatography-mass spectrometry (GC-MS) and Liquid chromatography-mass spectrometry (LC-MS/MS) techniques, the main degradation routes of atrazine are proposed.  相似文献   

3.
A photocatalyst based on CuO/SiO2 was prepared, and evaluated for the degradation of methylene blue in aqueous medium. The photocatalyst was obtained by calcination method of copper salt, in the presence of silica. The characterization by XRD, FTIR, and TPR techniques confirmed the formation of CuO as active phase. SEM studies showed CuO deposited on the surface of SiO2. By ESI-MS, it was demonstrated that the degradation of methylene blue occurs through successive hydroxylations. Photodegradation assays showed that CuO/SiO2 was efficient for degradation, and that the material worked better in the presence of UV light.  相似文献   

4.
We studied the hydrolysis of gas-phase carbon tetrachloride (CCl4), chloroform (CHCl3), and dichloromethane (CH2Cl2) over a metallic Fe surface for its application in combination with air stripping and soil vapour extraction. The effects of chlorocarbon concentration, type and preparation of the iron-containing material, humidity, and temperature on process performance are reported. The hydrolysis of chlorinated methane derivatives is catalysed by metallic iron resulting in a noticeable decrease of the reaction temperature. The reaction kinetics were found to be consistent with the Langmuir-Hinshelwood model.  相似文献   

5.
In this work, Er3+:YAlO3/TiO2 composite was synthesized by a ultrasonic dispersion and liquid boil method. The Er3+:YAlO3/TiO2 composite and pure TiO2 powder were characterized by XRD. The degradation of different organic dyes was used to evaluate the photocatalytic activity of the Er3+:YAlO3/TiO2 composite. It is found that the photocatalytic activity of Er3+:YAlO3/TiO2 composite is much higher than that for the similar system with only TiO2. Moreover, this Er3+:YAlO3/TiO2 composite provides a new way to take advantage of TiO2 in sewage treatment aspects using solar light.  相似文献   

6.
N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalysts, Pt/BaO/Al2O3, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al2O3 + Pd/Al2O3) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al2O3) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H2/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H2-TPR techniques. In addition, temperature programmed reactions of NO with H2/CO were conducted to obtain further information about N2O formation mechanism. Compared with Pt/BaO/Al2O3, (Pt/BaO/ Al2O3 + Pd/Al2O3) produced less N2O and more NH3 during NO x storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al2O3 + Al2O3). Temperature programmed reactions of NO with H2/CO results showed that Pd/Al2O3 component in (Pt/BaO/Al2O3 + Pd/Al2O3) played an important role in NO reduction to NH3, and the formed NH3 could reduce NO x to N2 leading to a decrease in N2O formation. Most of N2O formed over (Pt-Pd/BaO/Al2O3 + Al2O3) was originated from Pd/BaO/Al2O3 component. H2-TPR results indicated Pd-Ba interaction resulted in more difficultto- reduce PdOx species over Pd/BaO/Al2O3, which inhibits the NO dissociation and thus drives the selectivity to N2O in NO reduction.
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7.
We have discovered that HNO3 and related species are released from the TiO2 surface into air in the TiO2 photocatalytic oxidation of NO2 (1 ppm) under continuous UV light illumination (1 mW cm−2) by dehumidifying the outlet gas of the reaction and analyzing the recovered condensate liquid by ion chromatography. The origin of the HNO3 recovered in the dehumidifier could not be explained by a simple desorption of HNO3 overproduced on the TiO2 surface. The produced HNO3 must be activated on the TiO2 surface and causing the unidentified reaction.  相似文献   

8.
Bi2WO6 was synthesized with a hydrothermal method at different pHs and used for the degradation of tetracycline (TC) in water. The mesoporous Bi2WO6 prepared at pH 1 (BWO-1) displayed the highest adsorption and degradation capacity to TC due to its large surface area and more efficient capacity to separate photogenerated electrons and holes. 97% of TC at 20 mg·L?1 was removed by BWO-1 at 0.5 g·L?1 after 120 min irradiation under simulated solar light. Only 31% of the total organic carbon (TOC) was removed after 360 min irradiation although the TC removal reached 100%, suggesting that TC was mainly transformed to intermediate products rather than completely mineralized. The intermediates were identified by high-performance liquid chromatography-time of flight-mass spectrometry (HPLC-TOF-MS) and possible photodegradation pathways were proposed.  相似文献   

9.
Highly symmetrical molecules such as CH4, CF4 or SF6 are known to be atmospheric pollutants and greenhouse gases. High-resolution spectroscopy in the infrared is particularly suitable for the monitoring of gas concentration and radiative transfers in the earth's atmosphere. This technique requires extensive theoretical studies for the modeling of the spectra of such molecules (positions, intensities and shapes of absorption lines). Here, we have developed powerful tools for the analysis and the simulation of absorption spectra of highly symmetrical molecules. These tools have been implemented in the spherical top data system (STDS) and highly-spherical top data system (HTDS) software available at http://www.u-bourgogne.fr/LPUB/shTDS.html. They include a compilation of modeled data obtained during the last 20 years. An overview of our latest results in this domain will be presented. Electronic Publication  相似文献   

10.
Photocatalytic oxidation using semiconductors is one of the advanced oxidation processes for degradation of organic pollutants in water and air. TiO2 is an excellent photocatalyst that can mineralize a large range of organic pollutants such as pesticides and dyes. The main challenge is to improve the efficiency of the TiO2 photocatalyst and to extend TiO2 light absorption spectra to the visible region. A potential solution is to couple TiO2 with a narrow band gap semiconductor possessing a higher conduction band such as bismuth oxide. Therefore, here we prepared Bi2O3/TiO2 heterojunctions by the impregnation method with different Bi/Ti ratio. The prepared composites have been characterized by UV–Vis diffused reflectance spectra and X-ray diffraction. The photocatalytic activity of the heterojunction has been determined from the degradation of orange II under visible and UV light. Results show that Bi2O3/TiO2 heterojunctions are more effective than pure TiO2-anatase under UV-A irradiation, with an optimum for the Bi/Ti ratio of 5 %, for the photocatalytic degradation of Orange II. However, the photocatalytic activity under irradiation at λ higher than 420 nm is not much improved. Under UV–visible radiation, the two semiconductors are activated. We propose a mechanism explaining why our products are more effective under UV–visible irradiation. In this case the charge separation is enhanced because a part of photogenerated electrons from the conduction band of TiO2 will go to the conduction band of bismuth oxide. In this composite, titanium dioxide is the main photocatalyst, while bismuth oxide acts as adsorbent photosensitizer under visible light.  相似文献   

11.
Heterogeneous Fenton-like reaction has been extensively investigated to eliminate refractory organic contaminants in wastewater, but it usually shows low catalytic performance due to difficulty in reduction from Fe(III) to Fe(II). In this study, enhanced catalytic efficiency was obtained by employing Cu-doped BiFeO3 as heterogeneous Fenton-like catalysts, which exhibited higher catalytic performance toward the activation of H2O2 for phenol degradation than un-doped BiFeO3. BiFe0.8Cu0.2O3 displayed the best performance, which yielded 91% removal of phenol (10 mg L–1) in 120 min. The pseudo first-order kinetic rate constant of phenol degradation in BiFe0.8Cu0.2O3 catalyzed heterogeneous Fenton-like reaction was 5 times higher than those of traditional heterogeneous Fenton-like catalysts, such as Fe3O4 and goethite. The phenol degradation efficiency could still reach 83% after 4 cycles, which implied the good stability of BiFe0.8Cu0.2O3. The high catalytic activity of BiFe0.8Cu0.2O3 was attributed to the fact that the doping Cu into BiFeO3 could promote the generation of Fe(II) in the catalyst and then facilitate the activation of H2O2 to degrade the organic pollutants.
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12.
The transformation of the fungicide carbendazim (methyl-2 benzimidazole carbamate) induced by hydroxyl radical generated by the UV photolysis of H2O2 has been studied in dilute aqueous solution. The efficient reaction of hydroxyl radicals with carbendazim led to the rapid degradation of carbendazim. The study of reaction kinetics yielded a second order rate constant of 2.2±0.3 109 M−1 s−1 for HO· radicals with carbendazim. This value is in agreement with a high reactivity of HO· radicals with carbendazim. Most degradation products were identified by high performance liquid chromatography mass spectrometry (HPLC-MS). In the presence of hydrogenocarbonate and carbonate ions, hydroxyl radicals were quenched and in turn carbonate radicals CO3 ·− were formed. Carbonate radicals are indeed known to react efficiently with compounds containing electron-rich sites such as nitrogen or sulfur atoms. The use of a kinetic modelling software gave evidence for the occurrence of such reactions with carbendazim. The second order rate constant of carbonate radical with carbendazim was equal to 6±2 106 M−1 s−1. Electronic Publication  相似文献   

13.
The photodegradation of Acid blue 74 in aqueous solution employing a H2O2/ultraviolet system in a photochemical reactor was investigated. The kinetics of decolorization were studied by application of a kinetic model. The results show that the reaction of decolorization followed pseudo-first order kinetics. We demonstrate that there is an optimum H2O2 concentration, at which the rate of the decolorization reaction is maximum. Irradiation at 253.7 nm of the dye solution in the presence of H2O2 results in complete discoloration after ten minutes of treatment.  相似文献   

14.
A new type of Au/TiO2/reduced graphene oxide (RGO) nanocomposite was fabricated by the hydrothermal synthesis of TiO2 on graphene oxide followed by the photodeposition of Au nanoparticles. Transmission electron microscopy images showed that Au nanoparticles were loaded onto the surface of both TiO2 and RGO. Au/TiO2/RGO had a better photocatalytic activity than Au/ TiO2 for the degradation of phenol. Electrochemical measurements indicated that Au/TiO2/RGO had an improved charge transfer capability. Meanwhile, chemiluminescent analysis and electron spin resonance spectroscopy revealed that Au/TiO2/RGO displayed high production of hydrogen peroxide and hydroxyl radicals in the photocatalytic process. This high photocatalytic performance was achieved via the addition of RGO in Au/TiO2/RGO, where RGO served not only as a catalyst support to provide more sites for the deposition of Au nanoparticles but also as a collector to accept electrons from TiO2 to effectively reduce photogenerated charge recombination.
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15.
Chromium oxide and manganese oxide promoted ZrO2-CeO2 catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO x with NH3. A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H2 temperatureprogrammed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH3-SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO2-CeO2 binary oxide for the low temperature NH3-SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO2 and H2O. Cr-Zr-Ce mixed oxide exhibited>80% NO x conversion at a wide temperature window of 100°C–300°C. In situ DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr6 +. The present mixed oxide can be a candidate for the low temperature abatement of NO x .
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16.
Agricultural soils are an important source of greenhouse gases (GHG). Biochar application to such soils has the potential of mitigating global anthropogenic GHG emissions. Under irrigation, the topsoils in arid regions experience repeated drying and wetting during the crop growing season. Biochar incorporation into these soils would change the soil microbial environment and hence affect GHG emissions. Little information, however, is available regarding the effect of biochar addition on carbon dioxide (CO2) and nitrous oxide (N2O) emissions from agricultural soils undergoing repeated drying and wetting. Here, we report the results of a 49-day aerobic incubation experiment, incorporating biochar into an anthropogenic alluvial soil in an arid region of Xinjiang Province, China, and measuring CO2 and N2O emissions. Under both drying–wetting and constantly moist conditions, biochar amendment significantly increased cumulative CO2 emission. At the same time, there was a significant reduction (up to ~20 %) in cumulative N2O emission, indicating that the addition of biochar to irrigated agricultural soils may effectively slow down global warming in arid regions of China.  相似文献   

17.
In this study, FeVO4 was prepared and used as Fenton-like catalyst to degrade orange G (OG) dye. The removal of OG in an aqueous solution containing 0.5 g·L–1 FeVO4 and 15 mmol·L–1 hydrogen peroxide at pH 7.0 reached 93.2%. Similar rates were achieved at pH 5.7 (k = 0.0471 min–1), pH 7.0 (k = 0.0438 min–1), and pH 7.7 (k = 0.0434 min–1). The FeVO4 catalyst successfully overcomes the problem faced in the heterogeneous Fenton process, i.e., the narrow working pH range. The data for the removal of OG in FeVO4 systems containing H2O2 conform to the Langmuir–Hinshelwood model (R2 = 0.9988), indicating that adsorption and surface reaction are the two basic mechanisms for OG removal in the FeVO4–H2O2 system. Furthermore, the irradiation of FeVO4 by visible light significantly increases the degradation rate of OG, which is attributed to the enhanced rates of the iron cycles and vanadium cycles.
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18.
The photocatalytic degradation of a sulfonylurea herbicide, cinosulfuron, has been studied in TiO2 aqueous suspensions. A first order kinetic law was found. The influence of the initial concentration of cinosulfuron and of the initial radiant flux on the kinetics were evaluated. The identification of the intermediate products was based on high performance liquid chromatography coupled with mass spectrometry analyses (HPLC-MS). The mineralization of cinosulfuron was traced using ion chromatography and total organic carbon (TOC) measurements. These results indicate that the photocatalytic degradation of cinosulfuron leads to CO2, NO3 and SO4 2− as final products, and in addition cyanuric acid (C3H3O3N3), confirming previous results on triazinic ring-containing compounds. Electronic Publication  相似文献   

19.
Reductive dechlorination of chlorobenzene by Fe/ZrO2 in supercritical water was investigated. The effects of the operation conditions were studied. The dechlorination of chlorobenzene obeyed pseudo-first-order kinetics models. In supercritical water, the rate constant increases more rapidly with temperature than those in subcritical water. The results showed that the rate-determining step of dechlorination in subcritical water is diffusion; whereas the rate-determining of dechlorination in supercritical water is chemical reaction. The reaction mechanism in subcritical water might involve with an ionic mechanism; whereas the reaction mechanism in supercritical water might involve with a homolytic reaction.  相似文献   

20.
Multi-walled carbon nanotubes (MWCNTs)/TiO2 composite photocatalysts with high photoactivity were prepared by sol-gel process and further characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR), and UV-vis absorption spectra. Compared to pure TiO2, the combination of MWCNTs with titania could cause a significant absorption shift toward the visible region. The photocatalytic performances of the MWCNTs/TiO2 composite catalysts were evaluated for the decomposition of Reactive light yellow K-6G (K-6G) and Mordant black 7 (MB 7) azo dyes solution under solar light irradiation. The results showed that the addition of MWCNTs enhanced the adsorption and photocatalytic activity of TiO2 for the degradation of azo dyes K-6G and MB 7. The effect of MWCNTs content, catalyst dosage, pH, and initial dye concentration were examined as operational parameters. The kinetics of photocatalytic degradation of two dyes was found to follow a pseudo-first-order rate law. The photocatalyst was used for seven cycles with photocatalytic degradation efficiency still higher than 98%. A plausible mechanism is also proposed and discussed on the basis of experimental results.  相似文献   

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