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1.
A novel visible‐light‐driven g‐C3N4/MIL‐53(Al) composite photocatalyst was successfully prepared using a facile stirring method at room temperature. The g‐C3N4/MIL‐53(Al) composites were characterized and their effects on the photocatalytic activities for rhodamine B degradation were investigated. The g‐C3N4(20 wt%)/MIL‐53(Al) photocatalyst displayed optimal photocatalytic degradation efficiency, which was about five times higher than the photocatalytic activity of pure g‐C3N4. The improved photocatalytic performance of the g‐C3N4/MIL‐53(Al) photocatalyst was predominantly attributed to the efficient separation of electron–hole pairs and the low charge‐transfer resistance. g‐C3N4/MIL‐53(Al) also exhibited excellent stability and reusability. A proposed mechanism for the enhanced photocatalytic activity is also discussed based on the experimental results. Copyright © 2015 John Wiley & Sons, Ltd.  相似文献   

2.
The Fe3O4/TiO2/Bi2O3 composites were synthesized by a sol–gel method and used as improved photocatalysts for the degradation of methyl orange (MO) under simulated sunlight at room temperature. The as-prepared Fe3O4/TiO2/Bi2O3 composites were characterized by X-ray diffraction, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and diffuse reflectance spectroscopy (DRS). TEM analysis reveals that the composite has a core–shell structure and diameters of Fe3O4 core is about 200 nm. DRS results reveal that all composites showed red shift in optical absorption. TiO2, Fe3O4, and Bi2O3 exist mainly as separate phases in the Fe3O4/TiO2/Bi2O3 composites based on XPS analysis. The photocatalytic degradation of MO with the prepared photocatalysts was studied under simulated sunlight illumination. Photocatalytic reactivity test indicated that the removal efficiency of MO with the Fe3O4/TiO2/Bi2O3 photocatalyst was higher than that of pure TiO2 and Fe3O4/TiO2. Recovery rate of Fe3O4/TiO2/Bi2O3 photocatalysts achieved 80 % after five times reuse.  相似文献   

3.
Novel inorganic–organic yolk–shell microspheres based on Preyssler‐type NaP5W30O11014? polyoxometalate and MIL‐101(Cr) metal–organic framework (P5W30/MIL‐101(Cr)) were synthesized by reaction of K12.5Na1.5[NaP5W30O110], Cr(NO3)3·9H2O and terephthalic acid under hydrothermal conditions at 200°C for 24 h. The as‐prepared yolk–shell microspheres were fully characterized using various techniques. All analyses confirmed the incorporation of the Preyssler‐type NaP5W30O11014? polyoxometalate into the three‐dimensional porous MIL‐101(Cr) metal–organic framework. The results revealed that P5W30/MIL‐101(Cr) demonstrated rapid adsorption of cationic methylene blue (MB) and rhodamine B (RhB) with ultrahigh efficiency and capacity, as well as achieving rapid and highly selective adsorption of MB from MB/MO (MO = methyl orange), MB/RhB and MB/RhB/MO mixtures. The P5W30/MIL‐101(Cr) adsorbent not only exhibited a high adsorption capacity of 212 mg g?1, but also could quickly remove 100% of MB from a dye solution of 50 mg l?1 within 8 min. The effects of some key parameters such as adsorbent dosage, initial dye concentration and initial pH on dye adsorption were investigated in detail. The equilibrium adsorption data were better fitted by the Langmuir isotherm. The adsorption kinetics was well modelled using a pseudo‐second‐order model. Also, the inorganic–organic hybrid yolk–shell microspheres could be easily separated from the reaction system and reused up to four times without any change in structure or adsorption ability. The stability and robustness of the adsorbent were confirmed using various techniques.  相似文献   

4.
TiO2 and Fe-doped TiO2 thin films were prepared on the substrates (glass plates and glass microballs) after dipped in colloid and calcined at 500°C. The films have been characterized by UV-absorption, x-ray diffraction and atomic force microscopy (AFM). The investigated Fe-doped TiO2 (A nominal 10 wt% Fe2O3 was impregnated) thin films were obtained by sol-gel method. The characterization results suggest that the calcined thin films primarily consist of TiO2 anatase. And the light absorption curve of the TiO2 films modified with Fe showed that red shift had happened by the dope of Fe. TiO2/beads as photocatalyst were used to degrade the simulated dyeing water which contains reactive deep-blue dye (K-R). Through the degradation experiment, we found that the dope of Fe promoted the photocatalytic activities. The results showed that the dyeing water can be decomposed more effectively by the photocatalytic oxidation of Fe/TiO2 film on glass micro-balls than glass plates.  相似文献   

5.
Photocatalytic degradation of methyl orange (MO) as a model of an organic pollution was accomplished with magnetic and porous TiO2/ZnO/Fe3O4/PANI and ZnO/Fe3O4/PANI nanocomposites under visible light irradiation. The structures of nanocomposites were characterized by various techniques including UV–Vis absorption spectroscopy, XRD, SEM, EDS, BET and TGA. Optical absorption investigations show two λmax at 450 and 590 nm for TiO2/ZnO/Fe3O4/PANI nanocomposites respectively possessing optical band gaps about 2.75 and 2.1 eV smaller than that of the neat TiO2 and ZnO nanoparticles. Due to these optical absorptions, the nanocomposites can be considered promising candidates as visible light photocatalysts to produce more electron‐hole pairs. The degradation of MO, extremely increased using polymeric photocatalysts and decolorization in the presence of visible light achieved up to 90% in less than 20 min in comparison with the neat nanoparticles (about 10%). All these advantages promise a bright future for these composites as useful photocatalysts. The degradation efficiency of MO using stable nanocomposites was still over 70% after ten times reusing. The highest decolorizing efficiencies were achieved with 0.75 g L?1 of catalyst and 10 mg L?1 of MO at natural pH under visible light irradiation in less than 20 min.  相似文献   

6.
Excessive consumption of Fe (II) and massive generation of sludge containing Fe (III) from classic Fenton process remains a major obstacle for its poor recycling of Fe (III) to Fe (II). Therefore, the MHACF‐MIL‐101(Cr) system, by introducing H2, Pd0 and MIL‐101(Cr) into Fenton reaction system, was developed at normal temperature and pressure. In this system, the reduction of FeIII back to FeII by solid catalyst Pd/MIL‐101(Cr) for the storage and activation of H2, was accelerated significantly by above 10‐fold and 5‐fold controlled with the H2‐MIL‐101(Cr) system and H2‐Pd0 system, respectively. However, the concentration of Fe (II) generated by the reduction of Fe (III) could not be detected with the only input of H2 and without the addition of MOFs material. In addition, the apparent consumption of Fe (II) in MHACF‐MIL‐101(Cr) system was half of that in classical Fenton system, while more Fe (II) might be reused infinitely in fact. Accordingly, only trace amount of Fe (II) vs H2O2 concentration was needed and hydroxyl radicals through the detection of para‐hydroxybenzoic acid (p‐HBA) as the oxidative product of benzoic acid (BA) by·OH could be continuously generated for the effective degradation of 4‐chlorophenol(4‐CP). The effects of initial pH, concentration of 4‐CP, dosage of Fe2+, H2O2 and Pd/MIL‐101(Cr) catalyst, Pd content and H2 flow were investigated, combined with systematic controlled experiments. Moreover, the robustness and morphology change of Pd/MIL‐101(Cr) were thoroughly analyzed. This study enables better understanding of the H2‐mediated Fenton reaction enhanced by Pd/MIL‐101(Cr) and thus, will shed new light on how to accelerate Fe (III)/Fe (II) redox cycle and develop more efficient Fenton system.  相似文献   

7.
Photocatalysis provides a cost effective method for both renewable energy synthesis and environmental purification. Photocatalytic activity is dominated by the material design strategy and synthesis methods. Here, for the first time, we report very mild and effective photo‐deposition procedures for the synthesis of novel Fe2O3–TiO2 nanocomposites. Their photocatalytic activities have been found to be dramatically enhanced for both contaminant decomposition and photoelectrochemical water splitting. When used to decompose a model contaminant herbicide, 2,4‐dichlorophenoxyacetic acid (2,4‐D), monitored by both UV/Vis and total organic carbon (TOC) analysis, 10 % Fe–TiO2–H2O displayed a remarkable enhancement of more than 200 % in the kinetics of complete mineralisation in comparison to the commercial material P25 TiO2 photocatalyst. Furthermore, the photocurrent is nearly double that of P25. The mechanism for this improvement in activity was determined using density functional theory (DFT) and photoluminescence. These approaches ultimately reveal that the photoelectron transfer is from TiO2 to Fe2O3. This favours O2 reduction which is the rate‐determining step in photocatalytic environmental purification. This in situ charge separation also allows for facile migration of holes from the valence band of TiO2 to the surface for the expected oxidation reactions, leading to higher photocurrent and better photocatalytic activity.  相似文献   

8.
Sonophotocatalytic activity of methyl orange over Fe(III)/TiO2   总被引:1,自引:0,他引:1  
TiO2 doped with Fe3+ was prepared by an impregnation technique and its sonophotocatalytic activity over methyl orange (MO) was investigated. The Fe/TiO2 surface presented red shift to longer wavelength, resulting in a lower energy band gap. Fe loading of 0.1 wt% on TiO2 provided the optimum degradation. The MO degradation rate constant under sonophotocatalytic conditions was 2.5 times higher than under photocatalytic conditions.  相似文献   

9.
Nanocomposite of Fe3O4–nitrogen-doped graphene (Fe3O4–NG) was synthesized by single step hydrothermal method. The as-synthesized composite was characterised by various techniques such as powder X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, vibrating sample magnetometry and thermal analysis (TGA). The catalytic role of synthesized nanocomposite in visible light induced photodegradation of methyl orange (MO; acidic dye) and methylene blue (MB; basic dye) was explored. The role of Cu(II) ions on the photodegradation of the organic dyes was also monitored. Cu(II) ions enhance the photocatalytic activity of nanocomposite by capturing photoelectron, thereby quenching the recombination process of electron–hole pair in photocatalyst.  相似文献   

10.
In this work, the photocatalytic activity of the synthesized graphene oxide (GO)‐Fe3O4/TiO2 mesoporous photocatalysts was evaluated using chlorpyrifos (CP) as a contaminant. The nano‐photocatalyst was characterized by X‐ray diffraction, field emission scanning electron microscopy with energy‐dispersive X‐ray spectroscopy, transmission electron microscopy, and specific surface area by the Brunauer–Emmett–Teller method. Using visible light, the GO‐Fe3O4/TiO2 mesoporous photocatalyst was investigated on the degradation of CP pesticide. The GO‐Fe3O4/TiO2 photocatalyst displayed a good photocatalytic activity, which was achieving 97% of CP degradation after 60 min. Finally, experiments were performed to evaluate GO‐Fe3O4/TiO2 mesoporous nanocatalyst activity on repeated applications; after several uses, its photocatalytic activity was retained, which indicated stability.  相似文献   

11.
We proposed here a new process coupling dielectric barrier discharge (DBD) plasma with magnetic photocatalytic material nanoparticles for improving yield in DBD degradation of methyl orange (MO). TiO2 doped Fe3O4 (TiO2/Fe3O4) was prepared by the sol-gel method and used as a new type of magnetic photocatalyst in DBD system. It was found that the introduction of TiO2/Fe3O4 in DBD system could effectively make use of the energy generated in DBD process and improve hydroxyl radical contributed by the main surface Fenton reaction, photocatalytic reaction and catalytic decomposition of dissolved ozone. Most part of MO (88%) was degraded during 30 min at peak voltage of 13 kV and TiO2/Fe3O4 load of 100 mg/L, with a rate constant of 0.0731 min?1 and a degradation yield of 7.23 g/(kW h). The coupled system showed higher degradation efficiency for MO removal.  相似文献   

12.
《Arabian Journal of Chemistry》2020,13(11):8347-8360
FeN -co-doped TiO2 photocatalysts are prepared by sol–gel method using titanium tetraisopropoxide, urea and iron(II) acetylacetonate as precursors of titania, nitrogen and iron, respectively. The prepared samples are analysed from chemical-physical point of view by X-ray diffraction (XRD), Raman spectroscopy, UV–Vis diffuse reflectance spectroscopy (UV–Vis DRS), specific surface area measurements and scanning electron microscopy (FESEM). UV–Vis DRS spectra evidence that the co-doping of TiO2 with N and Fe leads to the narrowing of the band gap value (2.7 eV) with respect to Fe-doped TiO2 (2.8 eV) and N-doped TiO2 (2.9–3 eV). XRD patterns show that photocatalysts are mainly in anatase phase and Fe and N ions are successfully incorporated into the TiO2 lattice. The average crystallite size of Fe-N co-doped TiO2 is slightly lower than the other samples and equal to about 7 nm and the specific surface area of the co-doped sample results to be 117 m2 g−1. Photocatalytic performances of all prepared samples are evaluated by analysing the degradation of Acid Orange 7 azo dye under visible light irradiation. Photocatalytic efficiency obtained using FeN co-doped TiO2 strongly increases compared to undoped TiO2, N-doped TiO2 and Fe-doped TiO2 photocatalysts. In detail, using the co-doped photocatalyst, dye discoloration and mineralization result equal to about 90 and 83% after 60 min of LEDs visible light irradiation, underlining the best performances of the FeN co-doped TiO2 photocatalyst both in terms of treatment time and electric energy consumption.  相似文献   

13.
Fe-doped TiO2, Ti1–xFexO2 (x = 0.00, 0.02, 0.04, 0.06, 0.08, and 0.10), photocatalysts have been successfully synthesized via citric acid–assisted autocombustion method. The synthesized photocatalysts were characterized using different characterization techniques, such as X-ray diffraction (XRD), diffuse reflectance spectroscopy (DRS), Fourier transform infrared (FT-IR), transmission electron microscopy (TEM), energy dispersive x-ray spectroscopy (EDX), and x-ray photoelectron spectroscopy (XPS). The XRD diffraction patterns revealed that synthesized photocatalysts have the anatase phase of TiO2. The DRS analysis indicates a slight increment in absorbance in the visible light region by the Fe doping in TiO2. The FT-IR spectra reveal the various stretching and bending vibrational bands of the Ti–O lattice. The XPS spectra confirm the presence of elements titanium, oxygen, and iron in the synthesized samples and determine binding energy of elements. TEM analysis shows the shape of the synthesized photocatalyst, and it was used to calculate the average particle sizes of undoped and Fe-doped TiO2 (Ti0.96Fe0.04O2) photocatalysts using a histogram. The photocatalytic activities of synthesized photocatalysts were determined by photodegradation of dye (Direct Blue 199), contaminating carpet industry wastewater in the photochemical reactor and open pan reactor. The maximum photodegradation activity was shown by the Ti0.96Fe0.04O2 photocatalyst among all the synthesized undoped and Fe-doped photocatalysts. The synthesized photocatalyst (Ti0.96Fe0.04O2) had better photocatalytic activity when compared to both, undoped TiO2 and Aeroxide (Degussa) P-25. The used Fe-doped TiO2 photocatalyst (Ti0.96Fe0.04O2) was regenerated five times and investigated for its photocatalytic activity.  相似文献   

14.
In this work we synthesize a novel and highly efficient photocatalyst for degradation of methyl orange and rhodamine B. In addition, a new method for synthesis of Fe_3O_4@SiO_2@TiO_2@Ho magnetic core-shell nanoparticles with spherical morphology is proposed. The crystal structures, morphology and chemical properties of the as-synthesized nanoparticles were characterized using Fourier transform infrared spectroscopy(FT-IR), scanning electron microscopy(SEM), transmission electron microscopy(TEM), energy dispersive X-ray(EDS), X-ray diffraction(XRD), UV–vis diffuse reflectance spectroscopy(DRS) and vibrating sample magnetometer(VSM) techniques. The photocatalytic activity of Fe_3O_4@SiO_2@TiO_2@Ho was investigated by degradation of methyl orange(MO) as cationic dye and rhodamine B(Rh B) as anionic dye in aqueous solution under UV/vis irradiation. The results indicate that about 92.1% of Rh B and78.4% of MO were degraded after 120 and 150 min, respectively. These degradation results show that Fe_3O_4@SiO_2@TiO_2@Ho nanoparticles are better photocatalyst than Fe3O4@Si O2@TiO 2@Ho for degradation of MO and Rh B. As well as, the catalyst shows high recovery and stability even after several separation cycles.  相似文献   

15.
A precise fabrication of nanobamboo structures made from hybrid coordination polymers of the type {FexIn1?x}‐MIL‐88B is demonstrated. The compositions of the hybrid coordination polymer nanobamboos of {FexIn1?x}‐MIL‐88B (x=0.06, 0.19, or 0.75) are regulated by altering the amount of metal ions used in the reactions. Interestingly, the formation of a virtual In‐MIL‐88B (precise structure, {Fe0.06In0.94}‐MIL‐88B), which cannot be created in a typical reaction, is induced by the assistance of a Fe‐MIL‐88B structure. The a and c cell parameters of {Fe0.06In0.94}‐MIL‐88B are calculated at 10.95 and 19.86 Å, respectively. These values of {Fe0.06In0.94}‐MIL‐88B are larger than those of pure Fe‐MIL‐88B owing to the large ionic size of In3+ within the framework.  相似文献   

16.
Various polyoxometalates (POMs) were successfully immobilized to the mesoporous coordination polymer MIL‐101 resulting in a series of POM–MOF composite materials POM@MIL‐101 (POM=K4PW11VO40, H3PW12O40, K4SiW12O40). These materials were synthesized by a simple one‐pot reaction of Keggin POMs, tetramethylammonium hydroxide (TMAH), terephthalic acid (H2bdc), and Cr3+ ions. XRD, FTIR, thermogravimetric analyses (TG), inductively coupled plasma (ICP) spectrometry, and energy‐dispersive X‐ray spectroscopy (EDX) collectively confirmed the successful combination of POMs and the porous framework. Further, these composites POM@MIL‐101 with different loading of POMs were achieved by variation of the POM dosage. Notably, the uptake capacity of MIL‐101 towards organic pollutants in aqueous solution was significantly improved by immobilization of hydrophilic POMs into cages of MIL‐101. An uptake capacity of 371 mg g?1, comparable to that of the graphene oxide sponges, and much higher than that of the commercial activated carbon, was achieved at room temperature in 5 min when dipping 20 mg PW11V@MIL‐101 in the methylene blue (MB) solution (100 mL of 100 mg L?1 MB solution). Further study revealed that the POM@MIL‐101 composite materials not only exhibited a fast adsorption rate towards dye molecules, but also possessed of selective adsorption ability of the cationic dyes in wastewater. For example, the adsorption efficiency of PW11V@MIL‐101 (10 mg) towards MB (100 mL of 10 mg L?1) could reach 98 % in the initial 5 min, and it could capture MB dye molecules from the binary mixture of the MB and MO with similar size. Also, the POM@MIL‐101 materials could be readily recycled and reused, and no POM leached in the dye adsorption process.  相似文献   

17.
Dimethyldichlorosilane, one of the most consumed organosilicon monomers in the industry, can be prepared in a highly efficient and environmentally friendly synthesis method of disproportionating methylchlorosilanes. However, the internal mechanism of the reaction remains unclear. In this paper, the mechanism catalyzed by AlCl3/MIL‐53(Al) and AlCl3/MIL‐53(Al)@γ‐Al2O3 catalysts was calculated at B3LYP/6‐311++G(3df, 2pd) level by using the density functional theory (DFT). The results showed that although the two catalysts had similar active structures, the catalytic effects were significantly different. The Lewis acid center on the surface of γ‐Al2O3 in the core‐shell catalyst is complementary to the classic Lewis acid AlCl3 through the spatial superposition effect, which greatly improves the Lewis acid catalytic activity of AlCl3/MIL‐53(Al)@γ‐Al2O3.  相似文献   

18.
Photocatalysts with well‐designed compositions and structures are desirable for achieving highly efficient solar‐to‐chemical energy conversion. Heterostructured semiconductor photocatalysts with advanced hollow structures possess beneficial features for promoting the activity towards photocatalytic reactions. Here we develop a facile synthetic strategy for the fabrication of Fe2TiO5–TiO2 nanocages (NCs) as anode materials in photoelectrochemical (PEC) water splitting cells. A hydrothermal reaction is performed to transform MIL‐125(Ti) nanodisks (NDs) to Ti–Fe–O NCs, which are further converted to Fe2TiO5–TiO2 NCs through a post annealing process. Owing to the compositional and structural advantages, the heterostructured Fe2TiO5–TiO2 NCs show enhanced performance for PEC water oxidation compared with TiO2 NDs, Fe2TiO5 nanoparticles (NPs) and Fe2TiO5–TiO2 NPs.  相似文献   

19.
In this paper, TiO2 loaded on activated carbon fibers (ACF) was prepared by a coating treatment, followed by calcination at different temperatures in air atmosphere. The photocatalyst developed was characterized by SEM, XRD, XPS and UV-Vis adsorption spectroscopy. It was observed from SEM images that TiO2 loaded on ACF was in the form of small clusters with nanometer size. As confirmed by XRD and XPS determinations, the crystalline pattern of immobilized TiO2 was still anatase-form after calcination, and the micrographic structure and surface properties of ACF have not been damaged by the deposition process and calcination at different temperatures. Photocatalytic degradation of methylene blue (MB) in aqueous .solution was investigated using TiOE/ACF as photocatalyst. The comparison of photolysis, absorption and photocatalysis was carded out. The results indicated that the photocatalysis process of combined photocatalyst showed much higher degradation rate than that of photolysis and absorption processes. In addition, the possibility of cyclic usage of the photocatalyst was also confirmed.  相似文献   

20.
A magnetized nano‐photocatalyst based on TiO2/magnetic graphene was developed for efficient photodegradation of crystal violet (CV). Scanning electron microscopy, X‐ray diffraction, energy‐dispersive X‐ray spectroscopy and elemental mapping were used to characterize the prepared magnetic nano‐photocatalyst. The photocatalytic activity of the synthesized magnetic nano‐photocatalyst was evaluated using the decomposition of CV as a model organic pollutant under UV light irradiation. The obtained results showed that TiO2/magnetic graphene exhibited much higher photocatalytic performance than bare TiO2. Incorporation of graphene enhanced the activity of the prepared magnetic nano‐photocatalyst. TiO2/magnetic graphene can be easily separated from an aqueous solution by applying an external magnetic field. Effects of pH, magnetized nano‐photocatalyst dosage, UV light irradiation time, H2O2 amount and initial concentration of dye on the photodegradation efficiency were evaluated and optimized. Efficient photodegradation (>98%) of the selected dye under optimized conditions using the synthesized nano‐photocatalyst under UV light irradiation was achieved in 25 min. The prepared magnetic nano‐photocatalyst can be used in a wide pH range (4–10) for degradation of CV. The effects of scavengers, namely methanol (OH? scavenger), p‐benzoquinone (O2?? scavenger) and disodium ethylenediaminetetraacetate (hole scavenger), on CV photodegradation were investigated.  相似文献   

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