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1.
Tungsten and nitrogen co‐doped TiO2 nanobelts (W/N‐TNBs) have been successfully synthesized via 1‐step hydrothermal method. The structure, morphology, and composition of prepared samples were characterized by X‐ray diffraction, scanning electron microscopy, and X‐ray photoelectron spectroscopy, respectively. The prominent phase of all as‐prepared samples is anatase crystal. For samples with N doping, new energy states can be introduced on top of O 2p states which reduced the band gap by 1.1 eV. The reduced band gap leads to efficient visible light activity. The 3%‐W/N‐TNBs were found to exhibit the highest activity. The photocatalytic performance of 3%‐W/N‐TNBs under visible light is about 4.8 times than that of pure TiO2 nanobelts, which emphasizes the synergistic effect of W and N co‐doping for effectively inhibiting the recombination of photogenerated electrons and holes. In addition, our results testify the different redox potentials of the photoelectrons at different final states.  相似文献   

2.
TiO2 nanotubes (TiO2NTs) are beneficial for photogenerated electron separation in photocatalysis. In order to improve the utilization rate of TiO2NTs in the visible light region, an effective method is to use Aun cluster deposition-modified TiO2NTs. It is of great significance to investigate the mechanism of Aun clusters supported on TiO2NTs to strengthen its visible-light response. In this work, the structures, electronic properties, Mulliken atomic charge, density of states, band structure, and deformation density of Aun (n = 1, 8, 13) clusters supported on TiO2NTs were investigated by DMOL3. Based on published research results, the most stable adsorption configurations of Aun (n = 1, 8, 13) clusters supported with TiO2NTs were obtained. The adsorption energy increased as the number of Au adatoms increased linearly. The Aun clusters supported on TiO2NTs carry a negative charge. The band gaps of the three most stable structures of each adsorption system decreased compared to TiO2NTs; the valence top and the conduction bottom of the Fermi level come mainly from the contribution of 5d and 6s-Au. The electronic properties of the 5d and 6s impurity orbitals cause valence widening and band gap narrowing.  相似文献   

3.
Gold nanoparticle (Au‐NPs)‐Titanium oxide nanotube (TiO2‐NTs) electrodes are prepared by using galvanic deposition of gold nanoparticles on TiO2‐NTs electrodes as support. Scanning electron microscopy and energy‐dispersive X‐ray spectroscopy results indicate that nanotubular TiO2 layers consist of individual tubes of about 60–90 nm diameters and gold nanoparticles are well‐dispersed on the surface of TiO2‐NTs support. The electrooxidation of hydroquinone of Au‐NPs/TiO2‐NTs electrodes is investigated by different electrochemical methods. Au‐NPs/TiO2‐NTs electrode can be used repeatedly and exhibits stable electrocatalytic activity for the hydroquinone oxidation. Also, determination of hydroquinone in skin cream using this electrode was evaluated. Results were found to be satisfactory and no matrix effects are observed during the determination of hydroquinone content of the “skin cream” samples.  相似文献   

4.
A novel TiO2 nanotube array/CdS nanoparticle/ZnO nanorod (TiO2 NT/CdS/ZnO NR) photocatalyst was constructed which exhibited a wide‐absorption (200–535 nm) response in the UV/Vis region and was applied for the photoelectrocatalytic (PEC) degradation of dye wastewater. This was achieved by chemically assembling CdS into the TiO2 NTs and then constructing a ZnO NR layer on the TiO2 NT/CdS surface. Scanning electron microscopy (SEM) results showed that a new structure had been obtained. The TiO2 NTs looked like many “empty bottles” and the ZnO NR layer served as a big lid. Meanwhile the CdS NPs were encapsulated between them with good protection. After being sensitized by the CdS NPs, the absorption‐band edge of the obtained photocatalyst was obviously red‐shifted to the visible region, and the band gap was reduced from its original 3.20 eV to 2.32 eV. Photoelectric‐property tests indicated that the TiO2 NT/CdS/ZnO NR material maintained a very high PEC activity in both the ultraviolet (UV) and the visible region. The maximum photoelectric conversion efficiencies of TiO2 NT/CdS/ZnO NR were 31.8 and 5.98 % under UV light (365 nm) and visible light (420–800 nm), respectively. In the PEC oxidation, TiO2 NT/CdS/ZnO NR exhibited a higher removal ability for methyl orange (MO) and a high stability. The kinetic constants were 1.77×10?4 s?1 under UV light, which was almost 5.9 and 2.6 times of those on pure TiO2 NTs and TiO2 NT/ZnO NR, and 2.5×10?4 s?1 under visible light, 2.4 times those on TiO2 NT/CdS.  相似文献   

5.
A total of 35 [Au(NHC)2][MX2] (NHC=N‐heterocyclic carbene; M=Au or Cu; X=halide, cyanide or arylacetylide) complex salts were synthesized by co‐precipitation of [Au(NHC)2]+ cations and [MX2]? anions. These salts contain crystallographically determined polymeric Au???Au or Au???Cu interactions and are highly phosphorescent with quantum yields up to unity and emission color tunable in the entire visible regions. The nature of the emissive excited states is generally assigned to ligand (anion)‐to‐ligand (cation) charge‐transfer transitions assisted by d10???d10 metallophilicity. The emission properties can be further tuned by controlled triple‐component co‐crystallization or by epitaxial growth. Correct recipes for white light‐emitting phosphors with quantum yields higher than 70 % have been achieved by screening the combinatorial pool.  相似文献   

6.
N-doping of titania makes photocatalytic activity possible for the splitting of water, and other reactions, under visible light. Here, we show from both theory and experiment that Au preadsorption on TiO2 surfaces significantly increases the reachable amount of N implanted in the oxide. The stabilization of the embedded N is due to an electron transfer from the Au 6s levels toward the N 2p levels, which also increases the Au-surface adhesion energy. Theoretical calculations predict that Au can also stabilize embedded N in other metal oxides with photocatalytic activity, such as SrTiO3 and ZnO, producing new states above the valence band or below the conduction band of the oxide. In experiments, the Au/TiN(x)O(2-y) system was found to be more active for the dissociation of water than TiO2, Au/TiO2, or TiO(2-y). Furthermore, the Au/TiN(x)O(2-y) surfaces were able to catalyze the production of hydrogen through the water-gas shift reaction (WGS) at elevated temperatures (575-625 K), displaying a catalytic activity superior to that of pure copper (the most active metal catalysts for the WGS) or Cu nanoparticles supported on ZnO.  相似文献   

7.
TiO2 nanotubes were successfully co‐doped with sulfur and Ti3+ states using a facile annealing treatment in H2/H2S gas mixture. The obtained nanotubes were investigated for their photocatalytic performance and characterized by SEM, XRD, XPS, EPR, IPCE, IMPS and Mott‐Schottky measurements. The synthesized co‐doped TiO2 nanotubes show an enhanced photocatalytic hydrogen production rate compared to tubes that were treated only in pure H2 or H2S atmosphere—this without the presence of any co‐catalyst. It was found that sulfur in co‐doped TiO2 exists in the form of S2? and a small quantity of S4+/S6+, which leads to a narrowing of the band gap. However, the enhanced absorption of light in the visible range is not the key reason for the improved photocatalytic performance. We ascribe the enhanced photocatalytic activity to a synergetic effect of S mid‐gap states and disordered Ti3+ defects that facilitate photo generated electron transfer.  相似文献   

8.
Although TiO2 is an efficient photocatalyst, its large band gap limits its photocatalytic activity only to the ultraviolet region. An experimentally synthesized ternary Fe/C/S‐doped TiO2 anatase showed improved visible light photocatalytic activity. However, a theoretical study of the underlying mechanism of the enhanced photocatalytic activity and the interaction of ternary Fe/C/S‐doped TiO2 has not yet been investigated. In this study, the defect formation energy, electronic structure and optical property of TiO2 doped with Fe, C, and S are investigated in detail using the density functional theory + U method. The calculated band gap (3.21 eV) of TiO2 anatase agree well with the experimental band gap (3.20 eV). The defect formation energy shows that the co‐ and ternary‐doped systems are thermodynamically favorable under oxygen‐rich condition. Compared to the undoped TiO2, the absorption edge of the mono‐, co‐, and ternary‐doped TiO2 is significantly enhanced in the visible light region. We have shown that ternary doping with C, S, and Fe induces a clean band structure without any impurity states. Moreover, the ternary Fe/C/S‐doped TiO2 exhibit an enhanced photocatalytic activity, a smaller band gap and negative formation energy compared to the mono‐ and co‐doped systems. Moreover, the band edges of Fe/C/S‐doped TiO2 align well with the redox potentials of water, which shows that the ternary Fe/C/S‐doped TiO2 is promising photocatalysts to split water into hydrogen and oxygen. These findings rationalize the available experimental results and can assist the design of TiO2‐based photocatalyst materials.  相似文献   

9.
An investigation of hydrogen production with a series of Au/TiO2 photocatalysts reveals that the Au nanoparticles play different roles depending on the wavelength of the light irradiation. Under visible‐light irradiation, the photoactivity is primarily controlled by the intensity of the Au surface plasmon band, whereas under UV irradiation the Au nanoparticles act as co‐catalysts with TiO2.  相似文献   

10.
The energetic and electronic properties of N/V‐doped and N‐V‐codoped anatase TiO2 (101) surfaces are investigated by first‐principles calculations, with the aim to elucidate the relationship between the electronic structure and the photocatalytic performance of N‐V‐codoped TiO2. Several substitutional and interstitial configurations for the N and/or V impurities in the bulk phase and on the surface are studied, and the relative stability of different doping configurations is compared by the impurity formation energy. Systematic calculations reveal that N and V impurities can be encapsulated by TiO2 to form stable structures as a result of strong N‐V interactions both in the bulk and the surface model. Through analyzing and comparing the electronic structures of different doping systems, the synergistic doping effects are discussed in detail. Based on these discussions, we suggest that NOVTi codoping cannot only narrow the band gap of anatase TiO2, but also forms impurity states, which are propitious for the separation of photoexcited electron–hole pairs. In the case of NOVTi‐codoped TiO2 (101) surfaces, this phenomenon is especially prominent. Finally, a feasible synthesis route for NOVTi codoping into anatase TiO2 is proposed.  相似文献   

11.
采用水合肼(N2H4·H2O)作为还原剂,在液相环境中制备了自掺杂TiO2纳米管阵列(NTs)。利用FE-SEM、EDS、XPS、XRD、Raman、UV-Vis/NIR分光光度法以及半导体特性分析系统(Keithley 4200 SCS)分别对样品的形貌,晶体结构,光学特性以及电学性能进行了表征。结果表明:通过这种方法制备的自掺杂TiO2NTs在带隙中引入了大量的氧空位,创造了氧空位能级,从而提高了样品的电导率,有效提高光生电子-空穴对的产生、分离和传输。此外,由于氧空位的作用,使得TiO2NTs的带隙变窄,增强了可见光吸收能力,致使样品具有较高的光催化活性,并通过降解甲基橙溶液对样品的光催化活性进行评估。结果显示当光照150min后,自掺杂TiO2NTs对甲基橙溶液的降解率达73%,并且这种催化剂便于回收和重复使用。  相似文献   

12.
La-doped TiO2 nanotubes (La/TiO2 NTs) were prepared by the combination of sol-gel process with hydrothermal treatment. The prepared samples were characterized by using transmission electron microscopy, x-ray diffraction, x-ray photoelectron spectra, and ultraviolet-visible spectra. The photocatalytic performance of La/TiO2 NTs was studied by testing the degradation rate of methyl orange under ultraviolet (UV) irradiation. The results indicated La/TiO2 NTs calcined at 300°C consisted of anatase as the unique phase. The absorption spectra of the La/TiO2 NTs showed a stronger absorption in the UV range and a slight red shift in the band gap transition than that of pure TiO2 nanotubes. The photocatalytic performance of TiO2 NTs could be improved by the doping of lanthanum ions, which is ascribed to several beneficial effects the formation of Ti-O-La bond and charge imbalance, existing of oxygen defects and Ti3+ species, stronger absorption in the UV range and a slight red shift in the band gap transition, as well as higher equilibrium dark adsorption of methyl orange. 0.75 wt% La/TiO2 NTs had the best catalytic activity.  相似文献   

13.
Monodoping with Mo, Cr, and N atoms, and codoping with Mo?N and Cr?N atom pairs, are utilized to adjust the band structure of NaNbO3, so that NaNbO3 can effectively make use of visible light for the photocatalytic decomposition of water into hydrogen and oxygen, as determined by using the hybrid density functional. Codoping is energetically favorable compared with the corresponding monodoping, due to strong Coulombic interactions between the dopants and other atoms, and the effective band gap and stability for codoped systems increase with decreasing dopant concentration and the distance between dopants. The molybdenum, chromium, and nitrogen monodoped systems, as well as chromium–nitrogen codoped systems, are unsuitable for the photocatalytic decomposition of water by using visible light, because defects introduced by monodoping or the presence of unoccupied states above the Fermi level, which promotes electron–hole recombination processes, suppress their photocatalytic performance. The Mo?N codoped NaNbO3 sample is a promising photocatalyst for the decomposition of water by using visible light because Mo?N codoping can reduce the band gap to a suitable value with respect to the water redox level without introducing unoccupied states.  相似文献   

14.
We report the structural, thermal, optical, and redox properties of Fe‐doped cerium oxide (CeO2) nanoparticles, obtained using the polyol‐co‐precipitation process. X‐ray diffraction data reveal the formation of single‐phase structurally isomorphous CeO2. The presence of Fe3+ may act as electron acceptor and/or hole donor, facilitating longer lived charge carrier separation in Fe‐doped CeO2 nanoparticles as confirmed by optical band gap energy. The increased content of localized defect states in the ceria gap and corresponding shift of the optical absorption edge towards visible range in Fe‐doped samples can significantly improve the optical activity of nanocrystalline ceria. The better‐quality redox performances of the Fe‐doped CeO2 nanoparticles, compared with undoped CeO2 nanoparticles, were ascribed mainly to a decrease in band gap energy and an increase in specific surface area of the material. As observed from TPR studies all Fe ‐doped CeO2 nanoparticles, particularly the 10 mol % Fe doped CeO2 nanoproduct, exhibit excellent reduction performance.  相似文献   

15.
Introducing band gap states to TiO2 photocatalysts is an efficient strategy for expanding the range of accessible energy available in the solar spectrum. However, few approaches are able to introduce band gap states and improve photocatalytic performance simultaneously. Introducing band gap states by creating surface disorder can incapacitate reactivity where unambiguous adsorption sites are a prerequisite. An alternative method for introduction of band gap states is demonstrated in which selected heteroatoms are implanted at preferred surface sites. Theoretical prediction and experimental verification reveal that the implanted heteroatoms not only introduce band gap states without creating surface disorder, but also function as active sites for the CrVI reduction reaction. This promising approach may be applicable to the surfaces of other solar harvesting materials where engineered band gap states could be used to tune photophysical and ‐catalytic properties.  相似文献   

16.
The effect of N‐doping on the paramagnetic–antiferromagnetic transition associated with the metal–insulator (M–I) transition of V2O3 at 150 K has been studied in bulk samples as well as in nanosheets. The magnetic transition temperature of V2O3 is lowered to ~120 K in the N‐doped samples. Electrical resistivity data also indicate a similar lowering of the M–I transition temperature. First‐principles DFT calculations reveal that anionic (N) substitution and the accompanying oxygen vacancies reduce the energy of the high‐temperature metallic corundum phase relative to the monoclinic one leading to the observed reduction in Nèel temperature. In the electronic structure of N‐substituted V2O3, a sub‐band of 2p states of trivalent anion (N) associated with its strong bond with the vanadium cation appears at the top of the band of O(2p) states, the 3d‐states of V being slightly higher in energy. Its band gap is thus due to crystal field splitting of the degenerate d‐orbitals of vanadium and superexchange interaction, which reduces notably (ΔEg=?0.4 eV) due to their hybridization with the 2p states of nitrogen. A weak magnetic moment arises in the monoclinic phase of N‐substituted V2O3 with O‐vacancies, with a moment of ?1 μB/N localized on vanadium atoms in the vicinity of oxygen vacancies.  相似文献   

17.
In this work, CdS sensitized TiO2 nanotube arrays (CdS/TiO2NTs) electrode was synthesized with the CdS deposition on the highly ordered titanium dioxide nanotube arrays (TiO2NTs) by sequential chemical bath deposition method (S‐CBD). The as‐prepared CdS/TiO2NTs was characterized by field‐emission scanning electron microscopy (FE‐SEM) and X‐ray diffraction (XRD). The results indicated that the CdS nanoparticles were effectively deposited on the surface of TiO2NTs. The amperometric It curve on the CdS/TiO2NTs electrode was also presented. It was found that the photocurrent density was enhanced significantly from 0.5 to 1.85 mA/cm2 upon illumination with applied potential of 0.5 V at the central wavelength of 253.7 nm. The photoelectrocatalytic (PEC) activity of the CdS/TiO2NTs electrode was investigated by degradation of methyl orange (MO) in aqueous solution. Compared with TiO2NTs electrode, the degradation efficiencies of CdS/TiO2NTs electrode increased from 78% to 99.2% under UV light in 2 h, and from 14% to 99.2% under visible light in 3 h, which was caused by effective separation of the electrons and holes due to the effect of CdS, hence inhibiting the recombination of electron/hole pairs of TiO2NTs.  相似文献   

18.
In this study, we synthesized Tb/Tourmaline/TiO2 nano tubes (NTs) through a solgel-hydrothermal method. The as-prepared samples were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectromicroscope, scanning electron microscopy, transmission electron microscopy and UV-vis diffuse reflectance spectroscopy. The resulting Tb/Tourmaline/TiO2 NTs exhibited higher photocatalytic activity than pure TiO2 and TiO2 nano particles (NPs) in the degradation of menthyl orange under UV-light. Results revealed that doping rare earth element Tb could narrow the wide band gap of TiO2 and tourmaline could trap the photogenerated electron of TiO2 to inhibit the recombination of photogenerated electron-hole pairs.  相似文献   

19.
Doping is an efficient approach to narrow the band gap of TiO2 and enhance its photocatalytic activity. Here, we perform generalized gradient approximation (GGA)+U calculations to narrow the band gap of TiO2 by codoping of X (F, N) with transition metals (TM = Fe, Co) to extend the absorption edge to longer visible‐light wavelengths. Our results show that all the codoped systems can narrow the band gap significantly, in particular, (F+Fe)‐codoped system could serve as remarkably better photocatalysts with both narrowing of the band gap and relatively smaller formation energies than those of (F+Co) and (N+TM)‐codoped systems. Our results provide useful guidance for codoped TiO2 efficient for photocatalytic activity. © 2013 Wiley Periodicals, Inc.  相似文献   

20.
Nitrogen doped TiO2 represents one of the most promising material for photocatalitic degradation of environmental pollutants with visible light. However, at present, a great deal of activity is devoted to the anatase polymorph while few data about rutile are available. In the present paper we report an experimental characterization of N doped polycrystalline rutile TiO2 prepared via sol-gel synthesis. Nitrogen doping does not affect the valence band to conduction band separation but, generates intra band gap localized states which are responsible of the on set of visible light absorption. The intra band gap states correspond to a nitrogen containing defect similar but not coincident with that recently reported for N doped anatase.  相似文献   

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