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1.
A key to realizing the sustainable society is to develop highly active photocatalysts for selective organic synthesis effectively using sunlight as the energy source. Recently, metal‐oxide‐supported gold nanoparticles (NPs) have emerged as a new type of visible‐light photocatalysts driven by the excitation of localized surface plasmon resonance of Au NPs. Here we show that visible‐light irradiation (λ>430 nm) of TiO2‐supported Au NPs with a bimodal size distribution (BM‐Au/TiO2) gives rise to the long‐range (>40 nm) electron transport from about 14 small (ca. 2 nm) Au NPs to one large (ca. 9 nm) Au NP through the conduction band of TiO2. As a result of the enhancement of charge separation, BM‐Au/TiO2 exhibits a high level of visible‐light activity for the one‐step synthesis of azobenzenes from nitrobenzenes at 25 °C with a yield greater than 95 % and a selectivity greater than 99 %, whereas unimodal Au/TiO2 (UM‐Au/TiO2) is photocatalytically inactive.  相似文献   

2.
A facile method was used to prepare hollow mesoporous TiO2 and Au@TiO2 spheres using polystyrene (PS) templates. Au nanoparticles (NPs) were simultaneously synthesized and attached on the surface of PS spheres by reducing AuCl4? ions using sodium citrate which resulted in the uniform deposition of Au NPs. The outer coating of titania via sol‐gel produced PS@Au@TiO2 core–shell spheres. Removing the templates from these core–shell spheres through calcination produced hollow mesoporous and crystalline Au@TiO2 spheres with Au NPs inside the TiO2 shell in a single step. Anatase spheres with double Au NPs layers, one inside and another outside of TiO2 shell, were also prepared. Different characterization techniques indicated the hollow mesoporous and crystalline morphology of the prepared spheres with Au NPs. Hollow anatase spheres with Au NPs indicated enhanced harvesting of visible light and therefore demonstrated efficient catalytic activity toward the degradation of organic dyes under the irradiation of visible light as compared to bare TiO2 spheres.  相似文献   

3.
Uniform flower-like TiO2 coated Au nanostars and core-shell Au@Ag nanostars with different amounts of Ag coating were prepared through a facile method by hydrolysis of TiF4 under an acidic environment. The photocatalytic capability of these flower-like nanocomposites under visible light irradiation was found to be enhanced by up to 4.7-fold compared to commercial P25 TiO2 nanoparticles. The enhanced photocatalytic activity was ascribed to improved light absorption and hot electron injection from the photo-excited Au@Ag core to the TiO2 shell.  相似文献   

4.
A novel plasmonic photocatalyst, i.e., acid-etched TiO2 nanobelts attached with Ag/AgI nanoparticles (NPs) was prepared by deposition–precipitation-photoreduction method. Such surface-modified nanobelts had larger area than the normal one. Ag NPs were formed from AgI by photo-reduction under Xenon lamp irradiation. X-ray diffraction, scanning electron microscopy analysis, UV–Vis diffuse reflectance spectra and fluorescence spectra were used to characterize the structure and optical properties of the sample. The obtained sample exhibited strong photodegradation of methyl orange (MO) under visible light irradiation, which were attributed to both the surface plasmon resonance of Ag NPs and the visible light actived AgI. The photodegradation was accomplished by the transfer of photoexcited electrons from the Ag NPs to the acid-etched TiO2 nanobelts. After four cycles of photodegradation the photocatalyst was still stable. This novel photocatalyst had a high potential application in wastewater-treatment and biomedical engineering.  相似文献   

5.
Eco-friendly biosynthesis of polycrystalline titanium dioxide (TiO2) nanoparticles (NPs) was synthesised using Justicia gendarussa (J. gendarussa) leaf extract as oxidizing agents. They were compared with TiO2 NPs synthesized using the glacial acetic acid and also studied was the combined effect of synthesis of TiO2 NPs. The crystalline nature and structural formation of TiO2 NPs synthesized by different methods were confirmed by the X-ray diffraction technique, and functional groups of materials were confirmed by FT-IR spectroscopy. The synthesized materials were investigated for photocatalytic activity for methylene blue under UV irradiation and toxicity activity against MCF-7 and MDA-MB-231 cells. The result indicates that TiO2 NPs synthesised by J. gendarussa showed superior and enhanced activity against MCF-7 and MDA-MB-231. Biosynthesized TiO2 NPs showed higher photodegradation of dyes when compared with other TiO2 NPs synthesized by different methods. This is due to the alterations in band gap; structural changes and surface area in nanoparticles that increased the activity. Also, nanosphere/disc like morphology of TiO2 NPs is confirmed using TEM.  相似文献   

6.
One-dimensional (1D) Ag/AgBr/TiO2 nanofibres (NFs) have been successfully fabricated by the one-pot electrospinning method. In comparison with bare TiO2 NFs and Ag/AgBr/PVP (polyvinylpyrrolidone) NFs, the 1D Ag/AgBr/TiO2 NFs photocatalyst exhibits much higher photocatalytic activity in the degradation of a commonly used dye, methylene blue (MB), under visible light. The photocatalytic removal efficiency of MB over Ag/AgBr/TiO2 NFs achieves almost 100 % in 20 min. The photocatalytic reaction follows the first-order kinetics and the rate constant (k) for the degradation of MB by Ag/AgBr/TiO2 NFs is 5.2 times and 6.6 times that of Ag/AgBr/PVP NFs and TiO2 NFs, respectively. The enhanced photocatalytic activity is ascribed to the stronger visible light absorption, more effective separation of photogenerated electron-hole pairs, and faster charge transfer in the long nanofibrous structure. The Ag/AgBr/TiO2 NFs maintain a highly stable photocatalytic activity due to its good structural stability and the self-stability system of Ag/AgBr. The mechanisms for photocatalysis associated with Ag/AgBr/TiO2 NFs are proposed. The degradation of MB in the presence of scavengers reveals that h+ and ?O 2 ? significantly contribute to the degradation of MB.  相似文献   

7.
Co-doped BiVO4, a visible-light-responsive photocatalytic semiconductor, was synthesized using a microwave hydrothermal method. The doped sample exhibited much higher photocatalytic activity for malachite green degradation under visible light irradiation than undoped BiVO4. Similarly, improved inactivation efficiency toward Escherichia coli and Chlamydomonas pulsatilla (green tide) were observed with Co-doped BiVO4. The degradation of malachite green by Co-doped BiVO4 reaches 99% within 90 min irradiation to visible light. Similarly, the inactivation of Escherichia coli reaches 81.3% in 5 h and Chlamydomonas pulsatilla reaches 65.6% in 1 h irradiation to visible light. The enhanced photoactivity is believed to be due to the increment of the visible light absorption range by narrowing the band gap energy. In addition, the highly exposed reactive (010) facets can efficiently capture the photoinduced electrons, promote charge separation, and reduce recombination probability. Thus, these findings provide mechanistic insight into the effectiveness of Co-doped BiVO4 semiconductors for the treatment of wastewater that contains industrial effluents and microorganisms.  相似文献   

8.
In this work, we have prepared Al-doped TiO2 nanoparticles via a hydrothermal method and used it for making photoanode in dye-sensitized solar cell (DSSC). Material characterizations were done using XRD, AFM, SEM, TEM and EDAX. XPS results reveal that Al is introduced successfully into the structure of TiO2 creating new impurity energy levels in the forbidden gap. This resulted in tuning of the conduction band of TiO2 and reduced charge recombination which led to better current conversion efficiency of DSSC. Greater dye loading and enhanced surface area was obtained for Al-doped TiO2 compared to un-doped TiO2. I-V analysis, EIS and Bode plots are employed to evaluate photovoltaic performance. The short-circuit current density (J sc) and efficiency (η) of cell employing Al-doped TiO2 photoanode were extensively enhanced compared to the cell using un-doped TiO2. The optical band gap (E g) for Al-doped and un-doped TiO2 was obtained as 2.8 and 3.2 eV, respectively. J sc and η were 13.39 mAcm?2 and 4.27%, respectively, under illumination of 100 mWcm?2 light intensity when thin films of 1% Al-doped TiO2 was employed as photoanode in DSSC using N719 as the sensitizer dye. With the use of un-doped TiO2 as photoanode under similar conditions, J sc 5.12 mAcm?2 and η 1.06% only could be obtained. The maximum IPCE% obtained with Al-doped TiO2 and un-doped TiO2 was 67 and 38% respectively at the characteristic wavelength of dye (λ max = 540 nm). The EIS analyses revealed resistive and capacitive elements that provided an insight into various interfacial processes in terms of the charge transport. It was observed that Al-doping reduced the interfacial resistance leading to better charge transport which has improved both photocurrent density and conversion efficiency. Higher electron mobility and fast diffusion resulting in greater charge collection efficiency was obtained for Al-doped TiO2 compared to the un-doped TiO2. Using the Mott–Schottky plot, the donor density was calculated for un-doped and Al-doped TiO2. The work demonstrated that the Al-doped TiO2 is potential photoanode material for low-cost and high-efficiency DSSC.  相似文献   

9.
In this study, pure titanium dioxide (TiO2), Ta-doped TiO2, S-doped TiO2, and Ta-S-codoped rutile TiO2 photocatalysts were prepared by a sol-gel method. To evaluate the properties of the synthesized samples, X-ray diffraction analysis (XRD) and X-ray photoelectron spectroscopy (XPS) were applied. XRD detection results showed that the samples contained rutile phase basically. Scanning electron microscope observation showed that the morphology of Ta-S-TiO2 was nearly spherical. Transmission electron microscope investigation indicated that Ta-S-TiO2 had a flower-shaped structure consisting of many nanorods. The measurement of Brunauer-Emmett-Teller (BET)-specific surface areas (SBET) showed that tantalum and sulfur codoping can effectively increase the SBET of TiO2. XPS results indicated that Ta was in the form of Ta5+ in the TiO2 structure. Finally, the photocatalytic activities of synthesized photocatalyst samples were measured for the degradation of methylene blue in ultraviolet and visible light irradiation. The results demonstrated that the Ta-S-codoped rutile TiO2 photocatalyst had better photocatalytic performance than pure rutile TiO2, Ta-doped rutile TiO2 and S-doped rutile TiO2 photocatalyst.
Effects of pure TiO2, Ta-TiO2, S-TiO2, and Ta-S-TiO2 on degradation of MB under visible light irradiation (a) and ultraviolet (UV) irradiation (b) were studied. Ta-S-TiO2 exhibited a good photocatalytic performance under UV and visible light irradiation.
  相似文献   

10.
Three catalytic oxidation reactions have been studied: The ultraviolet (UV) light induced photocatalytic decomposition of the synthetic dye sulforhodamine B (SRB) in the presence of TiO2 nanostructures in water, together with two reactions employing Au/TiO2 nanostructure catalysts, namely, CO oxidation in air and the decomposition of formaldehyde under visible light irradiation. Four kinds of TiO2 nanotubes and nanorods with different phases and compositions were prepared for this study, and gold nanoparticle (Au‐NP) catalysts were supported on some of these TiO2 nanostructures (to form Au/TiO2 catalysts). FTIR emission spectroscopy (IES) measurements provided evidence that the order of the surface OH regeneration ability of the four types of TiO2 nanostructures studied gave the same trend as the catalytic activities of the TiO2 nanostructures or their respective Au/TiO2 catalysts for the three oxidation reactions. Both IES and X‐ray photoelectron spectroscopy (XPS) proved that anatase TiO2 had the strongest OH regeneration ability among the four types of TiO2 phases or compositions. Based on these results, a model for the surface OH group generation, absorption, and activation of molecular oxygen has been proposed: The oxygen vacancies at the bridging O2? sites on TiO2 surfaces dissociatively absorb water molecules to form OH groups that facilitate adsorption and activation of O2 molecules in nearby oxygen vacancies by lowering the absorption energy of molecular O2. A new mechanism for the photocatalytic formaldehyde decomposition with the Au/TiO2 catalysts is also proposed, based on the photocatalytic activity of the Au‐NPs under visible light. The Au‐NPs absorb the light owing to the surface plasmon resonance effect and mediate the electron transfers that the reaction needs.  相似文献   

11.
采用水热法以Hummers氧化法制备的氧化石墨和钛酸四丁酯为原料制备了部分还原的氧化石墨烯/二氧化钛(RGO/TiO2)复合光催化剂, 并研究了该复合材料在可见光以及紫外光下对亚甲基蓝的光催化降解活性.结果表明, 通过改变反应温度和氧化石墨加入量可以调控TiO2的晶相组成及其在复合材料中的分散性; 在水热反应过程中氧化石墨烯发生了部分还原; 所制备的RGO/TiO2复合材料的可见光和紫外光催化活性均高于纯TiO2; 部分还原的氧化石墨烯在复合材料中担当载体和电子受体, 同时可以使TiO2的初始吸收边向可见光区域红移, 增强了TiO2在可见光区域的吸收, 能有效提高对目标污染物的吸附性和光催化降解活性.  相似文献   

12.
A mesoporous iron–titanium mixed-oxides@activated carbon(AC) fiber membrane was fabricated by an electrospinning method and applied to the treatment of phenol waste water. The physical and chemical properties of the composite fiber membrane were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N2 adsorption/desorption, UV–Vis light diffuse reflectance spectroscopy (DRS), Raman spectroscopy, respectively. The results indicate that the composite nanofiber membrane is composed of α-Fe2O3, anatase TiO2 and activated carbon phases with a specific surface area of 231 m2 g–1 and narrow pore size distribution of 3–6 nm. DRS reveals that the composite membrane has high photons absorption from both ultraviolet light and visible light irradiation owing to the combination of Fe2O3, TiO2 and carbon. The prepared nano Fe2O3–TiO2@AC fiber membrane can act as an efficient reusable photocatalyst and adsorbent for 100% remo val of phenol pollutant. This hybrid technique is hopeful to be widely used in the treatment of various organic waste waters.  相似文献   

13.
Di(1H-tetrazol-5-yl)methane is employed as a new electron acceptor group in the synthesis of two metal-free organic dyes containing triphenylamine donor group. Dye-sensitized nanocrystalline TiO2 solar cell (DSSC) applying these novel dyes is constructed for consideration of their photovoltaic properties. The electronic properties of the dyes are also considered with the aid of theoretical calculations. The DSSC constructed from 4-(2,2-di(1H-tetrazol-5-yl)vinyl)-N,N-diphenylaniline (T1) shows a short-circuit photocurrent density of 13.38 mA cm?2, an open circuit voltage of 578 mV, and a fill factor of 0.54, with a resulted solar energy-to-electricity conversion efficiency of 4.18% under simulated 1 sun irradiation (100 mW cm?2). This result reveals that the dye with the di(1H-tetrazol-5-yl)methane anchoring group injects more electrons to the conduction band of TiO2 in comparison with its analogs with single tetrazole ring in their anchoring group. It is found that in spite of a red-shift of the absorption spectrum resulted from the lengthening of the molecule, the dye with two di(1H-tetrazol-5-yl)methane groups gives lower performance than the dye with a single electron acceptor.  相似文献   

14.
The large internal surface areas and outstanding electrical and mechanical properties of graphene have prompted to blend graphene with NiCo2O4 to fabricate nanostructured NiCo2O4/graphene composites for supercapacitor applications. The use of graphene as blending with NiCo2O4 enhances the specific capacitance and rate capability and improves the cyclic performance when compared to the pristine NiCo2O4 material. Here, we synthesized two different nanostructured morphologies of NiCo2O4 on graphene sheets by solvothermal method. It has been suggested that the morphologies of oxides are greatly influenced by dielectric constant, thermal conductivity, and viscosity of solvents employed during the synthesis. In order to test this concept, we have synthesized nanostructured NiCo2O4 on graphene sheets by facile solvothermal method using N-methyl pyrrolidone and N,N-dimethylformamide solvents with water. We find that mixture of N-methyl pyrrolidone and water solvent favored the formation of nanonet-like NiCo2O4/graphene (NiCoO-net) whereas mixture of N,N-dimethylformamide and water solvent produced microsphere-like NiCo2O4/graphene (NiCoO-sphere). Electrochemical pseudocapacitance behavior of the two NiCo2O4/graphene electrode materials was studied by cyclic voltammetry, chronopotentiometry, and electrochemical impedance spectroscopy techniques. The supercapacitance measurements on NiCoO-net and NiCoO-sphere electrodes showed specific capacitance values of 1060 and 855 F g?1, respectively, at the current density of 1.5 A g?1. The capacitance retention of NiCoO-net electrode is 93 % while that of NiCoO-sphere electrode is 77 % after long-term 5000 charge-discharge cycles at high current density of 10 A g?1.  相似文献   

15.
Almost vertically aligned ZnO nanowires have been grown on Silicon substrates via a simple hydrothermal method. In order to improve the photoelectric conversion efficiency for fabricated dye-sensitized solar cells (DSSCs), an easily-operated immersing method was employed to fabricate a TiO2/ZnO nanowires array heterojunction, which has advantage of high aspect ratio, low recombination rate and high absorption of visible light. The structure and surface morphology of the samples were characterized by X-ray powder diffraction (XRD) and scanning electron microscopy (SEM), respectively. The photovoltaic properties of TiO2/ZnO based DSCCs were measured by considering the power efficiency (η), photocurrent density (Jsc), open-circuit voltage (Voc), and fill factor (FF). An efficiency of 0.559% is achieved for the composite cell, increasing 0.426 and 0.185% for the ZnO nanowires cell and TiO2 cell, respectively. The short-circuit current and open-circuit voltage are also enhancing. The improvements are because of high surface are of TiO2 shell layer, as well as fast electron transport and light scattering effect of ZnO nanowires.  相似文献   

16.
Zero-dimensional (0D)/two-dimensional (2D) heterojunctions have attracted great attention in photocatalysis due to their superior interfacial effects. In this work, 0D g-C3N4 quantum dots (CNQDs) were firstly used to modify {001}-faceted 2D TiO2 nanosheets by a simple solvothermal method. During the controlled growth of TiO2 nanosheets with exposed reactive {001} facets, the CNQDs can be simultaneously assembled on the surface of TiO2 nanosheets in a highly dispersive way. The 0D/2D composite containing only 0.5% of CNQDs shows the optimized solar photocatalytic activity for the degradation of rhodamine B and 4-chlorophenol. More importantly, the 0D/2D composite exhibits a better solar photocatalytic activity than the bulk g-C3N4/TiO2 nanosheets composite. This improvement can be ascribed to the close interfacial contact and strong interaction between the highly dispersed CNQDs and the TiO2 nanosheets, which could lead to efficient separation of the photogenerated electron–hole pairs, provide more catalytic active sites, and enhance the absorption of solar light. The 0D/2D composite also shows good stability for its practical applications.  相似文献   

17.
As a typical photocatalyst for CO2 reduction, practical applications of TiO2 still suffer from low photocatalytic efficiency and limited visible‐light absorption. Herein, a novel Au‐nanoparticle (NP)‐decorated ordered mesoporous TiO2 (OMT) composite (OMT‐Au) was successfully fabricated, in which Au NPs were uniformly dispersed on the OMT. Due to the surface plasmon resonance (SPR) effect derived from the excited Au NPs, the TiO2 shows high photocatalytic performance for CO2 reduction under visible light. The ordered mesoporous TiO2 exhibits superior material and structure, with a high surface area that offers more catalytically active sites. More importantly, the three‐dimensional transport channels ensure the smooth flow of gas molecules, highly efficient CO2 adsorption, and the fast and steady transmission of hot electrons excited from the Au NPs, which lead to a further improvement in the photocatalytic performance. These results highlight the possibility of improving the photocatalysis for CO2 reduction under visible light by constructing OMT‐based Au‐SPR‐induced photocatalysts.  相似文献   

18.
The nanocomposites of titania coupled with graphene oxide (GO) and reduced graphene oxide (rGO), respectively, were prepared by homogeneous hydrolysis with urea. Graphene was obtained by effect of high‐intensity cavitation field on natural graphite in the presence of strong aprotic solvents in pressurized ultrasonic reactor. The morphology of TiO2–GO and TiO2–rGO composites was assessed by scanning electron microscopy and atomic force microscopy. The nitrogen adsorption–desorption was used for determination of surface area (BET) and porosity. Raman and IR spectroscopy were used for qualitative analysis and diffuse reflectance spectroscopy was employed to estimate band‐gap energies. Further enhancement of the photocatalytic activity was attained by codoping of composites with noble metals—Au, Pd and Pt. The photocatalytic activity of TiO2–GO and TiO2–rGO were assessed by photocatalytic decomposition of Orange II dye in an aqueous slurry under UV and visible light irradiation. The photocatalytic activity of noble metals codoped samples was determined with decomposition of Reactive Black 5 azo dye.  相似文献   

19.
In a tannic acid assisted synthesis of mesoporous TiO2, tannic acid was used as a cost effective and non‐toxic template for pore formation. Meanwhile, a gold nanoparticles (Au NPs) deposited TiO2 nanocomposite was coated on an indium tin oxide electrode for the fabrication of a photoelectrochemical (PEC) biosensing system. Upon the formation of anatase structure, the electrode was coated with MoS2 for effective visible light absorption. The mesoporous structure led to an enhanced surface area by improving Au NPs and glucose oxidase adsorption. Incorporation of Au NPs led to an enhanced photonic efficiency due to the generation of Schottky barriers. The obtained nanocomposite was used for the light‐driven, real‐time, and selective PEC glucose sensing. Under visible light irradiation, the enzyme immobilized electrodes yielded significant photocurrent improvement owing to the releasing electron donor H2O2. The obtained PEC biosensor demonstrated acceptable reproducibility and stability with a sensitivity of 4.42 μA mM?1 cm?2 and a low detection limit of 1.2 μM glucose. Also, the linear measurement range was found to be 0.004–1.75 mM glucose. The results indicated that the proposed production method of mesoporous TiO2 will pave the way for a green chemistry based porous material production, along with the extension of the implementation of semiconductors in PEC biosensing systems.  相似文献   

20.
We demonstrate the multiple plasmonic effect on the photocurrent properties of photoanodes containing Ag or Au nanoparticles (NPs) loaded onto titanium dioxide film (Ag–TiO2 or Au–TiO2) on Au grating surfaces. Ag–TiO2 or Au–TiO2 nanocomposite particles are prepared by a flame spray pyrolysis route. The structures and morphologies of the prepared products are characterized by high‐resolution transmission electron microscopy. The Ag–TiO2 or Au–TiO2 composite NPs are deposited by spin coating onto the Au grating surfaces. The photoanode electrode is a layered structure of blu‐ray disc‐recordable grating substrate/Au/Ag (or Au)–TiO2/dye/electrolyte/indium‐tin oxide. The plasmonic effect is induced when Ag or Au NPs are located within the propagating surface plasmon (SP) field on the Au grating surface. The short‐circuit photocurrent is increased by exciting the grating‐coupled propagating SP on the Au gratings and is further enhanced by positioning the Ag or Au NPs within the grating‐coupled SP field. Copyright © 2014 John Wiley & Sons, Ltd.  相似文献   

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