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1.
A novel compound, 5,7,14,16‐tetraphenyl‐8:9,12:13‐bisbenzo‐hexatwistacene ( TBH ), has been successfully synthesized through a retro‐Diels–Alder reaction. Single‐crystal structure analysis indicated that TBH has a twisted configuration with a torsion angle of 27.34°. The HOMO–LUMO gap of TBH calculated from the difference between the half‐wave redox potentials (E1/2ox=+0.40 eV and E1/2red=?1.78 eV) is 2.18 eV, which is in good agreement with the band gap (2.19 eV) derived from the UV/Vis absorption data. In addition, organic light‐emitting devices using TBH as emitter have been fabricated. The results revealed that TBH is a promising red light‐emitting candidate for applications in organic light‐emitting diodes.  相似文献   

2.
Photocatalytic processes triggered by graphene-based photocatalysts under solar light have sparked interest as a new sort of instrument for solar chemical synthesis. Herein we investigated self-assembled graphene quantum dots (GQDs)/NiSe-NiO composite photocatalyst for organic transformation as well as dye degradation. The synthesized GQDs/NiSe-NiO composite photocatalyst has an excellent suitable band gap, high molar extinction coefficient, low toxicity and chemical/thermal stability. The GQDs/NiSe-NiO composite photocatalyst emerges as a new standard for sulfur oxidation and dye degradation reactions under homemade LED light with high yield.  相似文献   

3.
Delafossite structured alpha-AgGaO(2) powder was successfully synthesized through a cation exchange reaction. alpha-AgGaO(2) has a band gap of 2.4 eV, absorbs visible light up to 520 nm, and effectively decomposes 2-propanol to CO2 via acetone by irradiating with either UV light (300-400 nm) or visible light (420-530 nm). The values of the quantum efficiency are similar (ca. 0.6%) under light irradiations with wavelengths of 365, 390, 430, 470, and 510 +/- 10 nm, but steeply decrease with wavelengths longer than 530 +/- 10 nm, which support a 2.4 eV band gap. In contrast, the other polymorph, alpha-AgGaO(2) powder, which has a band gap of 2.1 eV, shows a negligible activity when irradiating with either UV light or visible light. The higher oxidation activity of alpha-AgGaO(2) is probably due to its larger band gap, which is formed at the top of its valence band in a lower energy region as compared to alpha-AgGaO(2). Moreover, the first-principle calculations of alpha-AgGaO(2) and alpha-AgGaO(2) clearly indicate that alpha-AgGaO(2) has a remarkably larger dispersed valence band as compared to alpha-AgGaO(2), which is advantageous to the photocatalytic activity due to the efficient hole conduction.  相似文献   

4.
To investigate the role of oxygen defects on the photocatalytic activity of TiO2, the TiO2 nanocrystals with/without oxygen defects are successfully synthesized by the hydrothermal and sol-gel methods, respectively. The as-prepared TiO2 nanocrystals with defects are light blue and the absorption edge of light is towards the visible light region (~420 nm). Raman and X-ray photoelectron spectroscopy (XPS) measurements all confirm that the concentration of oxygen vacancies in the TiO2 synthesized by the sol-gel method is less than that synthesized through the hydrothermal route. The introduction of oxygen defects contributes to a new state in the band gap that narrows the band gap, which is the reason for the extension of light absorption into the visible light region. The photocurrent results confirm that this band-gap narrowing enhances the photocurrent response under simulated solar light irradiation. The TiO2 with oxygen defects shows a higher photocatalytic activity for decomposition of a methylene blue solution compared with that of the perfect TiO2 sample. The photocatalytic mechanism is discussed based on the density functional theory calculations and photoluminescence spectroscopy measurements.  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.
First-principles calculations were performed to study the structural and optoelectronic properties of the newly synthesized nonisovalent and lattice-matched (Si(2))(0.6)(AlP)(0.4) alloy (Watkins, T.; et al. J. Am. Chem. Soc.2011, 133, 16212). We found that the most stable structure of Si(3)AlP is a superlattice along the ?111? direction with separated AlP and Si layers, which has a similar optical absorption spectrum to silicon. The ordered C1c1-Si(3)AlP is found to be the most stable one among all structures with a basic unit of one P atom surrounded by three Si atoms and one Al atom, in agreement with experimental suggestions. (1) We predict that C1c1-Si(3)AlP has good optical properties, i.e., it has a larger fundamental band gap and a smaller direct band gap than Si; thus, it has much higher absorption in the visible light region. The calculated properties of Si(3)AlP suggest that it is a promising candidate for improving the performance of the existing Si-based solar cells. The understanding on the stability and band structure engineering obtained in this study is general and can be applied for future study of other nonisovalent and lattice-matched semiconductor alloys.  相似文献   

7.
A membrane‐intercalating conjugated oligoelectrolyte (COE), PTTP , was designed and synthesized with the goal of providing red‐shifted absorption spectra relative to previously synthesized COE analogs. Specifically, electron‐rich and electron‐poor subunits were introduced in the conjugated backbone to modulate the band gap. PTTP exhibits maxima of absorption at 507 nm and of emission at 725 nm. PTTP can also efficiently function to generate singlet oxygen in situ (ΦΔ≈20 %) and has appropriate topology and dimensions to interact with lipid membranes. The resulting rapid membrane insertion and sensitizing ability provide PTTP with a highly efficient antibacterial capability under a low light dose (0.6 J cm−2) toward Gram‐negative bacteria E. coli, making it a remarkably efficient optically mediated antimicrobial agent.  相似文献   

8.
We have synthesized new, efficient, visible light active photocatalysts through the incorporation of highly electronegative non-transition metal Pb or Sn ions into the perovskite lattice of Ba(In(1/3)Pb(1/3)M'(1/3))O3 (M = Sn, Pb; M' = Nb, Ta). X-ray diffraction, X-ray absorption spectroscopic, and energy dispersive spectroscopic microprobe analyses reveal that tetravalent Pb or Sn ions exist in the B-site of the perovskite lattice, along with In and Nb/Ta ions. According to diffuse UV-vis spectroscopic analysis, the Pb-containing quaternary metal oxides Ba(In(1/3)Pb(1/3)M'(1/3))O3 possess a much narrower band gap (E(g) approximately 1.48-1.50 eV) when compared to the ternary oxides Ba(In(1/2)M'(1/2))O3 (E(g) approximately 2.97-3.30 eV) and the Sn-containing Ba(In(1/3)Sn(1/3)M'(1/3))O3 derivatives (E(g) approximately 2.85-3.00 eV). Such a variation of band gap energy upon the substitution is attributable to the broadening of the conduction band caused by the dissimilar electronegativities of the B-site cations. In contrast to the ternary or the Sn-substituted quaternary compounds showing photocatalytic activity under UV-vis irradiation, the Ba(In(1/3)Pb(1/3)M'(1/3))O3 compounds induce an efficient photodegradation of 4-chlorophenol under visible light irradiation (lambda > 420 nm). The present results highlight that the substitution of electronegative non-transition metal cations can provide a very powerful way of developing efficient visible light harvesting photocatalysts through tuning of the band structure of a semiconductive metal oxide.  相似文献   

9.
Cu–1,4‐benzenedioxyacetic acid (Cu‐1,4‐BDOAH2) with a narrow band gap (2.52 eV) was synthesized and doped with Ce to afford Ce:Cu‐1,4‐BDOAH2 as an efficient photocatalyst with narrower band gap (2.39 eV). The prepared Cu‐1,4‐BDOAH2 and Ce:Cu‐1,4‐BDOAH2 were characterized using Fourier transform infrared, energy‐dispersive X‐ray, diffuse reflectance spectroscopies, scanning electron microscopy and X‐ray diffraction. The sonophotocatalytic degradation of diazinon was carried out in a batch‐mode reactor using visible light‐driven Ce:Cu‐1,4‐BDOAH2 photocatalyst as well as ultrasonic irradiation. The narrow band gap of the photocatalyst means that it can be activated under visible light illumination. The effects of operational parameters such as initial diazinon concentration (5–25 mg l?1), pH (2–10), photocatalyst dosage (10–30 mg) and irradiation time (10–30 min) on the sonophotocatalytic degradation efficiency were investigated using central composite design under response surface methodology. The optimization process was studied using desirability function and the results indicated 99.8% degradation, which was obtained at optimum values of 25 mg l?1, 6, 20 mg and 20 min for the initial concentration of diazinon, pH, photocatalyst dosage and irradiation time, respectively. Reusability experiments of Ce:Cu‐1,4‐BDOAH2 photocatalyst showed that it is quite stable with excellent catalytic activity even after five cycles.  相似文献   

10.
采用一步回流法制备了α-(Fe,Cu)OOH/RGO复合催化剂,通过粉末X射线衍射、扫描电子显微镜和X射线光电子能谱等对催化剂进行了表征,并以30 mg·L^-1的环丙沙星(CIP)为目标污染物,研究了不同制备条件下所得催化剂在可见光照射下协同H2O2对CIP的去除效果。结果表明,成功实现了α-(Fe,Cu)OOH纳米棒在石墨烯二维薄片上原位生长,α-(Fe,Cu)OOH/RGO复合材料的可见光吸收边发生红移,禁带宽度从2.02 eV变为1.76 eV。石墨烯复合不但增强了对污染物的吸附能力,而且加快了光生电子的分离、迁移速率,还提高了反应体系中电子的传导效率。当石墨烯复合比例(质量分数)为1%时,复合催化剂的催化性能最佳。当催化剂投加量为0.40 g·L^-1,H2O2浓度为0.10 mol·L^-1时,反应120 min,CIP被全部去除。α-(Fe,Cu)OOH/RGO循环使用5次,对CIP的去除率均在90%以上,表明催化剂具有较强的催化活性和较好的稳定性。  相似文献   

11.
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   

12.
CuO powders with a high specific surface area are shown to be able to produce H(2)O(2) in aqueous solution under simulated light irradiation. The highest rate of peroxide production was observed under mild experimental conditions using O(2) and a large surface area photocatalyst CuO irradiated with a solar simulator having light intensities between 60 and 90 mW/cm(2). The CuO employed had a specific surface area (SSA) of 64.8-70.1 m(2)/g and was prepared in a tubular furnace by controlled thermal decomposition of precipitated copper oxalate. The CuO particles produced were 1 mum cubes with primary particles around 15 nm. No peroxide was produced under the same conditions with commercial CuO, with SSA 200 times lower. The CuO synthesized during this work was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), specific surface area [Brunauer-Emmett-Teller (BET)], porosity, and X-ray photoelectron spectroscopy (XPS). From XPS, it was observed that only Cu(II) was present in the unused and used CuO. This indicates that the redox transient species involving other Cu oxidation states disappear very fast during the reaction, regenerating Cu(II) during H(2)O(2) production. Diverse experiments provided some evidence for the possible interfacial reaction mechanism leading to H(2)O(2), following the initial step of O(2)(-)(.) formation on the CuO surface under irradiation with photons, with energies exceeding the band gap of CuO. A photocatalyzed degradation of a concentrated 4-chlorophenol (4-CP) solution was observed under solar-simulated light in the presence of CuO.  相似文献   

13.
Carbon nitride(CN) photocatalysts have attracted much attention due to their excellent photocatalytic properties.And hydrothermal fluorination is a common method to improve the photocatalytic effect of CN photocatalyst.Here,the influence of the band gap was first revealed of fluorination and hydroxylation of CN photocatalyst based on the first theoretical principle.Here,the effect of fluorination and hydroxylation on the CN band gap was discussed for the first time using the first theoretical principle.With F atoms and OH doping,the band gap of CN was significantly improved,conduction band and valence band moved up.Then,F-CN photocatalyst with F atoms and OH was successfully synthesized by a hydrothermal fluorinated method.Next,the reasons why F-CN photocatalyst was more effective than that of traditional CN photocatalyst were fully discussed.From the photocatalytic effect of photocatalyst(12,593.2 μmolg-1 h-1to the morphology(super-small nanosheets),structure(homojunctions),composition(metal-free),specific surface area(54.1 m2/g),visible light absorption response(AQE is10.9% at 420 nm) and photo-induced carrier life(14.13 ns).Therefore,this work has a great guiding effect on the development of CN photocatalyst.  相似文献   

14.
层状纳米光催化复合材料HNbWO6/Pt的合成及性质   总被引:4,自引:0,他引:4  
用固相合成法合成出LiNbWO6,并用离子交换法制备出HNbWO6;通过PrNH2 层间膨胀、Pt(NH3 ) 2 + 4层间插入和紫外光分解等反应 ,合成出一种新的层状光催化纳米复合材料HNbWO6/Pt ,并比较了不同合成方法对样品性能的影响 .X射线衍射、漫反射、ICP和比表面积测定等的表征结果表明 :该样品的层间高度为 0 .3~ 0 .5nm ,禁带能隙为 2 .2 5~ 3.10eV .用波长大于 2 90nm的 45 0W汞灯照射 5h ,1g样品可催化分解甲醇溶液 (10 % )产生氢气约 40ml,表明所研制的层状纳米复合材料具有较高的光催化活性  相似文献   

15.
Surface water contamination by various dyes and pigments is a global problem caused by rapid industry, particularly textile/dyeing. Bangladesh's export-oriented textile sector has exploded in recent decades, polluting local waterways significantly. In this study, nano-ZnO were prepared using surfactant-assisted sol–gel, hydrothermal and thermal methods. SEM, XRD, reflectance spectrophotometer, EDS and adsorption tests were used to characterize the synthesized nano-ZnO. BET isotherms were used to determine the surface area, pore volume, and pore size of the as-prepared nano-ZnO. The mixed surfactant assisted-sol gel method produced nanorod-ZnO, whereas the hydrothermal and/or thermal methods yielded clusters of needles ZnO, as proven by SEM images. XRD data revealed that the synthesized nanorod-ZnO had a mainly wurtzite crystalline structure and their size was estimated using the Scherrer equation to be about 23.90 nm. EDS spectra confirmed the synthesis of pure nanorod-ZnO. Using a UV–visible reflectance spectrophotometer, the band gap energy of the as-prepared nanorod-ZnO was found to be 3.35 eV. According to BET isotherms, the BET and Langmuir surface areas were 4 and 5.4 m2/g, respectively. Prior to analyzing photodegradation, the RB was adsorbing in the presence of various doses of the nanorod-ZnO in the dark, but no adsorption was observed. The photocatalytic activities of the synthesized nano-ZnO were compared to TiO2 (anatase) for the degradation of RB in an aqueous system under solar light, UV, fluorescence, and tungsten filament light irradiation. Nanorod-ZnO showed exceptional photocatalytic activity in degrading RB in an aqueous solution under solar light irradiation. The results suggest that 0.01 g/50 mL nanorod-ZnO with a solution pH of 7.8 is the best combination for complete degradation of 2.00 × 10-5 M RB under solar light irradiation. When nano-ZnO was exposed to light, the inhibiting effect of ethanol and/or tert-butanol on the degradation of RB confirmed the formation of mostly hydroxyl free radicals. The synthesized nanorod-ZnO shown substantial photocatalytic activity in the removal of pollutants from industrial effluents and contaminated river water under solar light irradiation. A mechanism of excellent photocatalytic activity of the nanorod-ZnO is discussed.  相似文献   

16.
Ag-doped ZnO nanoparticles (Zn1?xAgxO; where x = 0.00–0.05) were synthesized by chemical precipitation method. The synthesized products were characterized by X-ray diffraction, scanning electron microscope (SEM), transmission electron microscope (TEM) and UV–Vis spectrometer. The SEM and TEM micrographs revealed the agglomerated spherical-like morphology and the measurements show that the size of crystallites is in the range of 10–40 nm. Optical measurements indicated a red shift in the absorption band edge after Ag doping. The band gap values of as prepared undoped and doped with silver samples were found to decrease with increase in temperature from 300 to 800 °C. Photocatalytic activities of ZnO and Ag doped ZnO were evaluated by irradiating the sample solution to ultraviolet light by taking methylene blue as organic dye. The experiment demonstrated that the photo-degradation efficiency of 1 mol% Ag-doped ZnO was significantly higher than that of undoped and 2–5 mol% Ag doped ZnO under ultraviolet light irradiation.  相似文献   

17.
Liu Y  Wei F  Yeo SN  Lee FM  Kloc C  Yan Q  Hng HH  Ma J  Zhang Q 《Inorganic chemistry》2012,51(8):4414-4416
A crystalline three-dimensional (3D) quaternary chalcohalide, Hg(7)InS(6)Cl(5) (1), has been synthesized through a solid-state reaction under medium temperature. It is the first example in the family of the Hg-IIIA-Q-X (Q = S, Se, Te; X = F, Cl, Br, I) systems. Compound 1 features a 3D network and has an optical band gap of 2.54 eV.  相似文献   

18.
Herein, we report visible light active mesoporous cadmium bismuth niobate(CBN) nanospheres as a photocatalyst for hydrogen(H_2) generation from copious hydrogen sulfide(H_2S). CBN has been synthesized by solid state reaction(SSR) and also using combustion method(CM) at relatively lower temperatures.The as-synthesized materials were characterized using different techniques. X-ray diffraction analysis shows the formation of single phase orthorhombic CBN. Field emission scanning electron microscopy and high resolution-transmission electron microscopy showed the particle size in the range of ~0.5–1 μm for CBN obtained by SSR and 50–70 nm size nanospheres using CM, respectively. Interestingly, nanospheres of size 50–70 nm self assembled with 5–7 nm nanoparticles were observed in case of CBN prepared by CM.The optical properties were studied using UV–visible diffuse reflectance spectroscopy and showed band gap around ~3.0 eV for SSR and 3.1 eV for CM. The slight shift in band gap of CM is due to nanocrystalline nature of material. Considering the band gap in visible region, the photocatalytic activity of CBN for hydrogen production from H_2S has been performed under visible light. CBN prepared by CM has shown utmost hydrogen evolution i.e. 6912 μmol/h/0.5 g which is much higher than CBN prepared using SSR.The enhanced photocatalytic property can be attributed to the smaller particle size, crystalline nature,high surface area and mesoporous structure of CBN prepared by combustion method. The catalyst was found to be stable, active and can be utilized for water splitting.  相似文献   

19.
A Bi-based oxychloride Bi(3)O(4)Cl with a layered structure as a novel efficient photocatalyst was studied in the present paper. The compound synthesized by a solid-state reaction method has a band gap of 2.79 eV. The material possesses a fair visible-light-induced photocatalytic activity. Generally, the photocatalytic efficiency of Bi(3)O(4)Cl for degrading methyl orange (MO) is higher than that of anatase TiO(2) under UV light illumination. The dispersion of Ag over Bi(3)O(4)Cl leads to an obvious increase in the photocatalytic performance. The MO decolorization over Bi(3)O(4)Cl is mainly initiated by a photocatalytic process. The photocatalytic activity is discussed in close connection with the crystal structure and the electronic structure in details.  相似文献   

20.
Metal oxide frame works along with carbon materials have been attracting tremendous attention of researches as the potential materials for energy and environmental remediation. In the present work heterostructures of (ZnO/CuO)/rGO ternary nanocomposites were synthesized by solid-state method. The crystalline structure of the nanoparticles was obtained from the XRD analysis. Optical band gap of the ZnO nanoparticles (3.1 eV) is tuned to 2.8 eV in the synthesized (ZnO/CuO)/rGO ternary nanocomposites. Field emission scanning electron microscope images of the (ZnO/CuO)/rGO ternary nanocomposites revealed formation of well-developed flowers like morphology of (ZnO/CuO) nanoparticles on rGO sheets. Photoluminescence spectroscopy analysis of (ZnO/CuO)/rGO ternary nanocomposites show enhancement in the electron-hole pair separation and thereby diminishing electron-hole pairs recombination rates effectively. In the present work, the photocatalytic activity of the ZC3G15 ternary nanocomposites show 99% and 93% of degradation efficiency respectively against RhB dye and 4-chlorophenol for 20 min under visible light irradiation. Thus, the simple solid-state method provides the effective ternary nanocomposites heterostructures light harvesting material for energy and environmental remediation.  相似文献   

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