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1.
Ag/AgBr/TiO2 was prepared by the deposition-precipitation method and was found to be a novel visible light driven photocatalyst. The catalyst showed high efficiency for the degradation of nonbiodegradable azodyes and the killing of Escherichia coli under visible light irradiation (lambda>420 nm). The catalyst activity was maintained effectively after successive cyclic experiments under UV or visible light irradiation without the destruction of AgBr. On the basis of the characterization of X-ray diffraction, X-ray photoelectron spectroscopy, and Auger electron spectroscopy, the surface Ag species mainly exist as Ag0 in the structure of all samples before and after reaction, and Ag0 species scavenged hVB+ and then trapped eCB- in the process of photocatalytic reaction, inhibiting the decomposition of AgBr. The studies of ESR and H2O2 formation revealed that *OH and O2*- were formed in visible light irradiated aqueous Ag/AgBr/TiO2 suspension, while there was no reactive oxygen species in the visible light irradiated Ag0/TiO2 system. The results indicate that AgBr is the main photoactive species for the destruction of azodyes and bacteria under visible light. In addition, the bactericidal efficiency and killing mechanism of Ag/AgBr/TiO2 under visible light irradiation are illustrated and discussed.  相似文献   

2.
Two series of nitrogen doped TiO(2) samples with different ratios of anatase to rutile phases were prepared by milling the mixture of P25 TiO(2) and C(6)H(12)N(4) in air and gaseous NH(3) atmosphere, respectively. Compared to air, NH(3) atmosphere plays an important role in delaying the crystallite transformation from anatase to rutile in the mechanochemical reaction of TiO(2) and C(6)H(12)N(4). In contrast to the previously reported results for pure TiO(2), it is found that nitrogen doped TiO(2) with higher content of rutile phase demonstrates higher photocatalytic activity in photodegrading pollutant Rhodamine B under both UV light and visible light irradiation (lambda>420 nm), and the amount of the surface-adsorbed water and hydroxyl groups on nitrogen doped TiO(2) have little correlations with their crystallite phases (anatase or rutile) and photocatalytic activity. The more abundant surface states characterized by photoluminescence spectroscopy together with the lowered valence band maximum of rutile TiO(2) by nitrogen doping are considered as the key factors for the higher activity of nitrogen doped TiO(2) with higher content of rutile phase.  相似文献   

3.
The Ce-TiO2 catalysts were prepared by controlled hydrolysis of Ti(OC(4)H(9))(4) with water generated "in situ" via an esterification reaction between acetic acid and ethanol, followed by hydrothermal treatment. The samples were characterized by X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (DRS), scanning electron microscopy (SEM), atomic absorption flame emission spectroscopy (AAS), and nitrogen adsorption-desorption methods. Both of undoped TiO2 and Ce-TiO2 samples exclusively consist of primary anatase crystallites, which further form spherical aggregates with diameters ranging from 100 to 500 nm. The photocatalytic activity of Ce-TiO2 was investigated for the photocatalytic degradation of Rhodamine B (RB) aqueous solution both under UV and visible light irradiation. Doping of Ce(4+) effectively improves the photocatalytic activity under both UV light irradiation and visible light irradiation with an optimal doping concentration of 0.2 and 0.4%, respectively. The photocatalytic mechanisms of Ce-TiO2 catalysts were tentatively discussed.  相似文献   

4.
Visible-light-driven TiO2 photocatalysts doped with nitrogen have been prepared as powders and thin films in a cylindrical tubular furnace under a stream of ammonia gas. The photocatalysts thus obtained were found to have a band-gap energy of 2.95 eV. Electron spin resonance (ESR) under irradiation with visible light (lambda > or = 430 nm) afforded the increase in intensity in the visible-light region. The concentration of trapped holes was about fourfold higher than that of trapped electrons. Nitrogen-doped TiO2 has been used to investigate mechanistically the photocatalytic oxidation of trichloroethylene (TCE) under irradiation with visible light (lambda > or = 420 nm). Cl and O radicals, which contribute significantly to the generation of dichloroacetyl chloride (DCAC) in the photocatalytic oxidation of TCE under UV irradiation, were found to be deactivated under irradiation with visible light. As the main by-product, only phosgene was detected in the photocatalytic oxidation of TCE under irradiation with visible light. Thus, the reaction mechanism of TCE photooxidation under irradiation with visible light clearly differs markedly from that under UV irradiation. Based on the results of the present study, we propose a new reaction mechanism and adsorbed species for the photocatalytic oxidation of TCE under irradiation with visible light. The energy band for TiO2 by doping with nitrogen may involve an isolated band above the valence band.  相似文献   

5.
Well-crystallized iron(III)-doped TiO2 nanopowders with controlled Fe3+ doping concentration and uniform dopant distribution, have been synthesized with plasma oxidative pyrolysis. The photocatalytic reactivity of the synthesized TiO2 nanopowders with a mean particle size of 50-70 nm was quantified in terms of the degradation rates of methyl orange (MO) in aqueous TiO2 suspension under UV (mainly 365 and 316 nm) and visible light irradiation (mainly 405 and 436 nm). The photodecomposition of MO over TiO2 nanopowders followed a distinct two-stage pseudo first order kinetics. Interestingly, the photocatalytic reactivity depends not only on the iron doping concentration but also on the wavelength of the irradiating light. Under UV irradiation, nominally undoped TiO2 had much higher reactivity than Fe3+ -doped TiO2, suggesting that Fe3+ doping (> 0.05 at. %) in TiO2 with a mean particle size of approximately 60 nm was detrimental to the photocatalytic decomposition of methyl orange. Whereas, under visible light irradiation, the Fe3+ -doped TiO2 with an intermediate iron doping concentration of approximately 1 at. % had the highest photocatalytic reactivity due to the narrowing of band gap so that it could effectively absorb the light with longer wavelength. A strategy for improving the photocatalytic reactivity of Fe3+ -doped TiO2 used in the visible light region is also proposed.  相似文献   

6.
Usually, SrTiO3 monodoped with Cr cations at the Ti4+ site hardly shows visible light photocatalytic activity. Revealing the origin of this issue is important for us to find an alternative approach to make SrTiO3 active under visible light irradiation. In this paper, two Cr-doped SrTiO3-(Sr0.95Cr0.05)TiO3 and Sr(Ti0.95Cr0.05)O3-were synthesized by a conventional solid-state reaction method, and their photophysical and photocatalytic properties were studied comparatively. It was found that both (Sr0.95Cr0.05)TiO3 and Sr(Ti0.95Cr0.05)O3 showed considerable absorption to visible light. However, their photocatalytic activities for H2 evolution from aqueous methanol solution under visible light irradiation were significantly different: the H2 evolution rate over (Sr0.95Cr0.05)TiO3 (approximately 21 micromol/h) was more than 100 times that over Sr(Ti0.95Cr0.05)O3 (approximately 0.2 micromol/h). X-ray photoelectron spectroscopy analysis results revealed that the Cr cations doped at the Sr2+ site were all trivalent state (Cr3+), while those doped at the Ti4+ site were mixed valent states (Cr3+ and Cr6+). The different photocatalytic activities of H2 evolution are supposed to closely relate to the different valent states of Cr doped at different sites (Sr2+ or Ti4+) in SrTiO3. Possible electronic structures of (Sr0.95Cr0.05)TiO3 and Sr(Ti0.95Cr0.05)O3 were proposed in relation to their photophysical and photocatalytic properties.  相似文献   

7.
Cerium-doped Titanium dioxide (TiO(2)) nanoparticles are prepared by sol-gel method. Doping shifts the UV absorption edge of TiO(2) to the visible region, making it efficient for visible light photocatalysis. Incorporation of cerium decreases the effective band gap of TiO(2) and increases the Urbach energy levels. At the dopant concentrations of 0.015 and 0.025 mol the luminescence intensity increases compared to undoped TiO(2); however, the luminescence is quenched at 0.035 mol. Quenching of luminescence indicates efficient separation of charge carriers. Undoped TiO(2) is showing poor performance in the photocatalytic degradation of methyl orange under visible light. However, on cerium doping its photoactivity is increased, and is drastically enhanced at 0.035 mol of cerium. Further increase in Ce(3+) doping level to 0.045 mol results in the reduction of the photodegradation of the dye. On UV irradiation, entire samples show good photocatalytic activity up to 30 min, but their efficiency decreases when irradiation time is increased to 45 min. Irradiation for longer time results in negative charging of the TiO(2) surface with migrating electrons. The negatively charged surface repels the OH(-) ion and O(2) molecule from adsorbing on its surface thus decreasing the availability of hydroxyl and superoxide radical for dye degradation.  相似文献   

8.
An ion-implantation method was used to prepare V-ion-implanted P25 TiO2 photocatalysts. Their photocatalytic activity for the degradation of formic acid under visible light irradiation (lambda>450 nm) was investigated. Upon implantation of V ions into the lattice of P25 TiO2, the photoactivity was remarkably enhanced. HRTEM images showed that the implanted V ions existed in the form of VO2(T) in the lattice of P25 TiO2. The intensity of photoluminescence (PL) spectra of V-ion-implanted P25 TiO2 decreased with the increase of the amount of implanted V ions, indicating the decrease of electron-hole pair recombination. It was also observed that the lower the PL intensity of V-ion-implanted P25 TiO2, the higher the photoactivity.  相似文献   

9.
Sulfur doped anatase TiO2 nanoparticles (3 nm−12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3M NaOH at room temperature. The electro-optical and photocatalytic properties of the synthesized sulfur doped TiO2 nanoparticles were studied along with Degussa commercial TiO2 particles (24 nm). The results show that band gap of TiO2 particles decreases from 3.31 to 3.25 eV and for that of commercial TiO2 to 3.2 eV when the particle sizes increased from 3 nm to 12 nm with increase in sulfur doping. The results of the photocatalytic activity under UV and sun radiation show maximum phenol conversion at the particle size of 4 nm at 4.80% S-doping. Similar results are obtained using UV energy for both phenol conversion and conversion of CO2+H2O in which formation of methanol, ethanol and proponal is observed. Production of methanol is also achieved on samples with a particle size of 8 and 12 nm and sulfur doping of 4.80% and 5.26%. For TiO2 particle of 4 nm without S doping, the production of methanol, ethanol and proponal was lower as compared to the S-doped particles. This is attributed to the combined electronic effect and band gap change, S dopant, specific surface area and the light source used.  相似文献   

10.
采用溶胶-凝胶法制备了Fe3+掺杂的Fe-K2La2Ti3O10光催化剂, 并通过X射线衍射(XRD)、紫外-可见漫反射(DRS)、X射线光电子能谱(XPS)等技术对其进行了表征和分析, 考察了不同掺杂量对K2La2Ti3O10的性质及光催化分解水制氢活性的影响. 结果表明, Fe-K2La2Ti3O10在400-650 nm范围内显示强吸收, 光谱响应扩展到可见光区(λ>400 nm), 掺杂Fe3+后, K2La2Ti3O10的可见光区的光催化制氢活性显著提高, 掺杂量为nFe/nTi=0.04时活性最佳, 当催化剂用量为0.1 g, 反应液为CH3OH(30 mL)+H2O(90 mL)时, 产氢量达到1.92 μmol·h-1, 为未掺杂时的4倍.  相似文献   

11.
为了改善纳米二氧化钛的光催化活性,通过水热法制备了氮钨共掺杂二氧化钛纳米棒。通过扫描电镜(SEM),X射线衍射(XRD),透射电镜(TEM),X射线光电子能谱(XPS)和紫外可见光吸收光谱 (UV-VIS)等对产物进行了相关表征。结果显示:与未掺杂的二氧化钛相比,氮钨共掺杂的二氧化钛纳米棒在可见光区域显示出了较强的光催化活性。因为氮钨阳离子的掺入拓宽了可见光的吸收区域。  相似文献   

12.
Transparent, ordered nanoporous TiO2/Al2O3 composite films doped with metal elements (Ru, Si, and Te) and nonmetal elements (N, C, and S) were fabricated by successive anodization and sol-gel process directly on glass substrates covered with a tin-doped indium oxide (ITO) film. The doping of ruthenium, nitrogen, carbon, and sulfur in TiO2 exhibited an enhanced effect on the absorbance, while the doping of silicon and tellurium showed little effect. Particularly, the N- and Ru-doped TiO2/Al2O3 films on ITO/glass developed an enhanced absorption red shift of 580 nm (-N) and 500 nm (-Ru). The nanoporous TiO2/Al2O3 composite film exhibited the highest photocatalytic activity in decomposing acetaldehyde under ultraviolet-light irradiation, with a value of 13 times in initial reaction rate or 7.8 times in quantum yield higher than a commercially available TiO2 material, Degussa P25. The ultraviolet-light photocatalytic activities of nanoporous TiO2/Al2O3 films were enhanced by the doping of nitrogen, carbon, and sulfur but slightly weakened by the doping of ruthenium, silicon, and tellurium. Particularly, the nanoporous N-doped TiO2/Al2O3 films exhibited effective photocatalytic activity on ultraviolet light decomposition of a highly toxic dioxin, HpCDD, and gave the highest decomposition rate of approximately 95% (via 7 h of irradiation) for the specimen with a dopant content of 1.7 wt % nitrogen.  相似文献   

13.
Nanocrystalline Ta(3)N(5) particles with a surface area of more than 33 m(2)/g were synthesized by nitridation of nanosized Ta(2)O(5) particles using NH(3) as the reactant gas. It was found that nanocrystalline Ta(2)O(5) was converted into Ta(3)N(5) completely (by X-ray diffraction, XRD) at 700 degrees C within 5.0 h, which was much lower than the temperature 900 degrees C for the complete nitridation of micrometer-sized Ta(2)O(5) powder. The oxide precursor and the resulting nitride were characterized by XRD analysis, transmission electron microscopy, UV-vis diffuse reflectance spectra, and BET surface area techniques. The nitrogen contents in the prepared Ta(3)N(5) powders were quantitatively determined with a CHN elemental analyzer. Nanocrystalline Ta(3)N(5) showed an absorption edge of around 600 nm, and Ta(3)N(5) in the size of about 26 nm exhibited a blue shift of 15 nm in the adsorption edge. The photocatalytic activity of the prepared Ta(3)N(5) under UV-vis and visible light irradiation was compared to that of nanocrystalline TiO(2-x)N(x) using the photocatalytic degradation of methylene blue (MB) as a model reaction. The Ta(3)N(5) nanoparticles showed the significantly enhanced photocatalytic activity for the degradation of MB in comparison with the larger-sized Ta(3)N(5). Moreover, the nanocrystalline Ta(3)N(5) showed much higher photocatalytic activity under visible light irradiation compared with TiO(2-x)N(x) in the same size.  相似文献   

14.
CdS-sensitized Pt/TiO(2) nanosheets with exposed (001) facets were prepared by hydrothermal treatment of a Ti(OC(4)H(9))(4)-HF-H(2)O mixed solution followed by photochemical reduction deposition of Pt nanoparticles (NPs) on TiO(2) nanosheets (TiO(2) NSs) and chemical bath deposition of CdS NPs on Pt/TiO(2) NSs, successively. The UV and visible-light driven photocatalytic activity of the as-prepared samples was evaluated by photocatalytic H(2) production from lactic acid aqueous solution under UV and visible-light (λ ≥ 420 nm) irradiation. It was shown that no photocatalytic H(2)-production activity was observed on the pure TiO(2) NSs under UV and/or visible-light irradiation. Deposition of CdS NPs on Pt/TiO(2) NSs caused significant enhancement of the UV and visible-light photocatalytic H(2)-production rates. The morphology of TiO(2) particles had also significant influence on the visible-light H(2)-production activity. Among TiO(2) NSs, P25 and the NPs studied, the CdS-sensitized Pt/TiO(2) NSs show the highest photocatalytic activity (13.9% apparent quantum efficiency obtained at 420 nm), exceeding that of CdS-sensitized Pt/P25 by 10.3% and that of Pt/NPs by 1.21%, which can be attributed to the combined effect of several factors including the presence of exposed (001) facets, surface fluorination and high specific surface area. After many replication experiments of the photocatalytic hydrogen production in the presence of lactic acid, the CdS-sensitized Pt/TiO(2) NSs did not show great loss in the photocatalytic activity, confirming that the CdS/Pt/TiO(2) NSs system is stable and not photocorroded.  相似文献   

15.
We report the photooxidation of toluene over nitrogen doped TiO(2) (TiO(2-x)N(x)) under visible light irradiation. The photocatalytic oxidation of toluene in air over TiO(2-x)N(x) powders was studied using diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS), gas chromatography (GC), ion chromatography (IC), and gas chromatography mass spectrometry (GC-MS), focusing on the photocatalytic decomposition processes of toluene. Results obtained indicate that toluene, weakly adsorbed on the catalyst surface, is initially photooxidized to benzaldehyde which adsorbs onto the TiO(2-x)N(x) surface more strongly, leading to the formation of ring-opening products such as carboxylic acids and aldehydes. No gaseous intermediates were detected during the photooxidation. Major intermediates adsorbed at the catalyst surface were oxalic acid, (COOH)(2), acetic acid, CH(3)COOH, formic acid, HCOOH, and pyruvic acid, CH(3)COCOOH, whereas more complicated carboxylic species, including propionic acid, CH(3)CH(2)COOH, isovaleric acid, (CH(3))(2)CHCH(2)COOH, and succinic acid, (CH(2)COOH)(2), were also found in the early stage of the photooxidation. These intermediate products were gradually photodegraded to CO(2) and H(2)O under visible light irradiation.  相似文献   

16.
In order to develop photoactive cobalt-doped TiO2 for the degradation of organic pollutants using visible light irradiation, the effects of cobalt precursor on TiO2 microstructure were investigated. Three cobaltprecursors, i.e. CoCl2, Co(NO3)2 and CoSO4 with two doping levels (nominally 1% and 10%), and two annealing temperatures (400 and 800 ℃) were adopted to prepare the doped titania through the sol-gel method. The powder samples were characterized with XRD, SEM, BET surface area analysis and UV-Vis absorption spectroscopy, and their photocatalytic activities were evaluated by the degradation of aniline under visible light irradiation. The results showed that the distribution of titania phases, particle size,morphology, surface area and the optical absorption of the catalysts were greatly dependent on the cobalt precursors. Samples prepared from Co(NO3)2, especially for those doped at 1% and calcined at 400 ℃,showed the highest photocatalytic activity towards the degradation of aniline, and the possible reasons are discussed briefly.  相似文献   

17.
采用非离子表面活性剂C18H37(OCH2CH2)10OH(Brij-76)作为模板剂, 在以杂多酸H6P2W18O62对TiO2掺杂改性基础上, 通过模板-溶胶-凝胶-程序升温溶剂热一步法在较低温度下制备了有序复合介孔材料H6P2W18O62/TiO2(Brij-76). 通过傅立叶变换红外(FT-IR)光谱, X射线衍射(XRD), 扫描电子显微镜(SEM), 能量色散X射线(EDX), N2吸附-脱附测定和NH3程序升温脱附(NH3-TPD)等手段对其进行了表征. 结果表明, 以非离子表面活性剂Brij-76为模板剂制得的复合材料H6P2W18O62/TiO2(Brij-76)平均孔径约为3.31 nm, BET比表面积为99.78 m2·g-1. 与TiO2相比, 其孔径有序性大幅度提高, 粒子的聚集度降低, 表面酸性显著增加. 微波增强光催化性能研究结果显示, H6P2W18O62/TiO2(Brij-76)在微波作用下催化活性更高, 可有效地降解一氯苯溶液.  相似文献   

18.
N掺杂纳米TiO2可见光催化氧化丙烯的动力学行为   总被引:1,自引:0,他引:1  
通过在不同温度的氨气气氛中处理纳米管钛酸(NTA)制得具有可见光响应的氮掺杂纳米二氧化钛. X射线衍射(XRD)谱表征结果显示, 当温度高于400 ℃时, 样品由正交晶系向锐钛矿相转变, 700 ℃处理得到的样品除了锐钛矿相TiO2外还有TiN 新相存在; 紫外-可见扩散漫反射(DRS)结果表明, 氮掺杂纳米TiO2在整个可见光区都有明显的吸收. 不同波长可见光及不同气体流速的光催化氧化丙烯动力学研究表明, 活性最好的N掺杂纳米TiO2催化剂(600 ℃ NH3处理)对可见光的利用范围可扩展至500 nm, 低浓度丙烯光催化氧化反应为一级反应.  相似文献   

19.
通过水热方法合成了可见光响应的LaVO4/TiO2纳米管, 采用XRD, TEM, 氮气吸附-脱附以及表面光电压谱对样品进行了表征. 以气相甲苯为典型污染物, 研究了制备样品在可见光(λ>420 nm)条件下的光催化性能. 实验结果表明, LaVO4的复合使TiO2的粒径减小, 比表面积增大, 光响应范围向可见光偏移. 光催化实验结果表明, 在可见光条件下, LaVO4/TiO2纳米管降解甲苯的效率比其它样品高, 与纯TiO2纳米管相比, 降解效率提高了47%.  相似文献   

20.
TiO2因其毒性低、稳定性高、制备成本低廉而获得广泛应用,特别是作为光催化剂在降解环境污染物方面受到了广泛关注;然而,纯TiO2较大的光生载流子复合率和较宽的带隙限制了其应用.元素掺杂作为一种拓宽光催化剂光吸收能力的方法广泛应用于各种光催化剂的修饰改性,而两种具有光催化性能的TiO2相共存则能有效抑制光生载流子的复合,因此采取合适的方法有效利用这两种TiO2改性的方法制备得到更具实际应用潜质的光催化剂具有一定的可行性.本文通过简单的溶胶-凝胶过程向锐钛矿相与金红石相组成的混相TiO2中共掺杂碳和钇得到了一种活性较高的可见光响应光催化剂.采用粉末X射线衍射、拉曼光谱、X射线光电子能谱和透射电镜等表征手段研究了碳和钇掺杂对TiO2结构的影响,发现碳掺杂有利于金红石相的形成且材料具有更大的晶粒尺寸,钇掺杂则有利于锐钛矿相的形成且能细化材料的晶粒尺寸,提高材料的比表面积,导致材料更好的光催化活性.材料在30 W荧光灯光照条件下的光催化降解亚甲基蓝(MB)性能的研究显示,C-Y-TiO2样品具有比单掺杂和未掺杂样品更高的光催化活性,其顺序为C-Y-TiO2>Y-TiO2>C-TiO2>TiO2≈P25.此外,降解反应动力学研究表明C-Y-TiO2样品光降解MB的速率是未掺杂样品在相同条件下降解速率的3.5倍.不同钇掺杂含量样品的结构和光催化降解MB的研究结果表明,钇掺杂显著促进了锐钛矿相TiO2的形成.这说明钇可能仅掺杂进入锐钛矿相,因此合适的钇掺杂量才能有效形成最优化的光催化性能的混相TiO2.不同热处理温度下获得的样品的光降解MB特性也表明,一定的热处理温度有利于合适的锐钛矿相和金红石相的组成,从而有利于相间的协同效应.紫外-可见光谱和荧光光谱表征分析表明,碳和钇的掺杂都拓展了其吸收光谱到可见光区域,且抑制了光生电子和空穴对的复合,进而提高了材料的光催化活性.碳和钇共掺杂的混相TiO2具有较高可见光光催化活性的主要原因有两个方面:一是元素掺杂减小了TiO2的带隙使得材料具有可见光响应;二是金属和非金属元素在锐钛矿相与金红石相TiO2中不同的掺杂特性形成的协同效应,抑制了光生电子和空穴的复合.  相似文献   

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