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1.
Developing new renewable, carbon-neutral fuels to diminish the amount of released CO2 in the atmosphere and to solve global challenges such as global warming and climate change is significant. Among them, hydrogen (H2) is attracting much attention due to its high energy density, ease of transportation, and multiple means of production. To meet the global demand of H2, photocatalytic water splitting is one of the most promising methods for large scale production. Herein, Al-doped SrTiO3 photocatalyst (Al–SrTiO3) was prepared by a molten flux method. Then, plasmonic metal nanoparticles (Au, Cu, Pt), and cocatalysts Rh/Cr2O3 and CoOOH were selectively deposited onto the reductive and oxidative active sites of Al–SrTiO3 using multi-step photodeposition-impregnation methods for water splitting and H2 production under UV-rays, UV–Vis. Light, and visible light (λ ≥ 400 nm). Our results showed that, compared with Pt and Cu loaded Al–SrTiO3 photocatalyst supported with Rh/Cr2O3 and CoOOH cocatalysts, Au-loaded samples showed the highest H2 production efficiency under both UV (920 μmol/h - EQE = 41% at 365 nm) and UV–Vis (100.5 μmol/h) rays. In addition, the amount of evolved H2 decreased by increasing the weight ratio of Au nanoparticles (NPs) due to the overlap between Au NPs and Rh/Cr2O3 cocatalyst. Although Au 0.3 wt%-loaded sample showed high activity under both UV and UV–Vis. Rays, it exhibited almost no efficiency under visible light because of the large bandgap of Al–SrTiO3 (3.1 eV) and the poor absorption in the visible region. Visible light absorption was then enhanced by increasing the loaded amount of Au NPs and by separating Au NPs and Rh/Cr2O3 cocatalyst responsible for H2 evolution by combining both photodeposition and impregnation methods. Under visible light, Rh/Cr2O3-loaded Al–SrTiO3 with 4 wt % Au NPs showed the highest H2 evolution efficiency (41 μmol/3 h). This was attributed to the efficient hot electron transfer from Au NPs to Al–SrTiO3 then to RhCr2O3, resulting in charge separation needed for efficient H2 generation.  相似文献   

2.
An efficient visible light responsive photocatalyst Ce/N co-doped SrTiO3 was prepared via a hydrothermal method for hydrogen production. The phase structure, morphology, contents and valence states of the dopant elements, specific surface area, optical properties, and photocatalytic activity of the samples were characterized. The transient photocurrent response and electrochemical impedance spectra under visible light illumination indicated that Ce/N co-doped SrTiO3 possessed a more intense photo-current response and lower surface resistance than N–SrTiO3 and Ce–SrTiO3. The water splitting rate of Ce/N-co-doped SrTiO3 is 4.28 mmol/g/h, which is 84.49 times higher than that of pure SrTiO3. The enhanced photocatalytic performance is due to the narrowing of the band gap of SrTiO3 by Ce ion and N ion impurities.  相似文献   

3.
An effective improvement of hydrogen evolution from water splitting under solar light irradiation was investigated using quantum dots (QDs) compounds loaded onto a Au/TiO2 photocatalyst. First, Au/TiO2 was prepared by the deposition-precipitation method, and then sulfide QDs were loaded onto the as-prepared Au/TiO2 by a hydrothermal method. QDs were loaded onto Au/TiO2 to enhance the energy capture of visible light and near-infrared light of the solar spectrum. The results indicated that the as-prepared heterojunction photocatalysts absorbed the energy from the range of ultraviolet light to the near-infrared light region and effectively reduced the electron-hole pair recombination during the photocatalytic reaction. Using a hydrothermal temperature of 120 °C, the as-prepared (ZnS–PbS)/Au/TiO2 photocatalyst had a PbS QDs particle size of 5 nm, exhibited an energy gap of 0.92 eV, and demonstrated the best hydrogen production rate. Additionally, after adding 20 wt % methanol as a sacrificial reagent to photocatalyze for 5 h, the hydrogen production rate reached 5011 μmol g−1 h−1.  相似文献   

4.
Photocatalyst Bi1−xSmxVO4 were prepared by solid phase reaction and characterized by XRD, UV–visible DRS, BET, and SEM. Bi1−xSmxVO4 showed two structures with the component content. When the composition was above x = 0.3, Bi1−xSmxVO4 were of single phase with tetragonal type and can be regarded as solid solutions of was BiVO4 and SmVO4. When Bi1−xSmxVO4 was loaded with 0.3 wt% Pt, the samples showed photocatalytic activities for water decomposition to hydrogen under UV light. Among these catalysts, Bi0.5Sm0.5VO4 showed the best photocatalytic activity for water splitting, which indicated synergistic of Bi/Sm enhanced the photocatalysis efficiency. What's more, Bi0.5Sm0.5VO4 loaded with other co-catalysts was found to act as a photocatalyst for water decomposition to hydrogen and oxygen under UV light irradiation, and the photocatalyst loaded with Pt/Cr2O3 had the best photocatalytic property. The amounts of the produced hydrogen and oxygen, respectively, were about 188.25 μmol h−1 g−1 and 95.90 μmol h−1 g−1. This study indicated that the formation of solid solution was the feasible method to adjust energy band and synergistic of Bi/Sm can enhance the photocatalytic activities of water decomposition.  相似文献   

5.
The organic-inorganic composite g-C3N4–SrTiO3:Rh was prepared for the first time as a photocatalyst for hydrogen production and the resulting hydrogen evolution rate under visible light irradiation from aqueous methanol solution was measured. A high hydrogen evolution rate of 223.3 μmol h−1 was achieved by using 0.1 g of as-prepared photocatalyst powder comprised of 20 wt.% g-C3N4 80 wt.% SrTiO3:Rh (0.3 mol%). The hydrogen evolution rate was greater than that obtained by SrTiO3:Rh (0.3 mol%) by a factor of 3.24. The quantum efficiency of as-prepared composite photocatalyst was 5.5% at 410 nm for hydrogen evolution. The high activity of the composite photocatalyst for hydrogen evolution stemmed from its electron–hole separation and transportation capabilities due to the hetero-junctions of the organic-inorganic composite materials. The proposed mechanism for the electron–hole separation and hydrogen evolution of the g-C3N4–SrTiO3:Rh composite under visible light irradiation featured the reduced recombination of the photo-generated charge carriers. The doping of Rh ions into the SrTiO3 has contributed to the high photocatalytic activity by forming a donor level from the valance band to the conduction band.  相似文献   

6.
The enhanced photocatalytic hydrogen production from aqueous methanol solution using ZnO was investigated with aid of simultaneous metal deposition. The simultaneous deposition for such metals as Ag, Au, Cu, Ni, Pd, Pt, and Rh was evaluated for the H2 production from aqueous methanol solution. As a result, the addition of Cu ion was effective improvement in photocatalytic hydrogen evolution. The photocatalytic hydrogen production using ZnO photocatalyst with aid of simultaneous deposition of Cu was approximately 130 times better than those obtained with bare ZnO. The Cu-deposited ZnO had the response to the visible light for the hydrogen formation. After the photocatalytic hydrogen production, the in-situ Cu-photodeposited ZnO sample was characterized by X-ray diffraction (XRD), UV–visible diffuse reflectance spectrometry (UV-DRS), and photoluminescence (PL) spectroscopy.  相似文献   

7.
Nitrogen/titanium dioxide (N/TiO2) visible light photocatalysts were prepared using the sol–gel method. The catalysts were characterized using transmission electron microscopy, reflective UV–visible spectroscopy, specific surface area measurements, and X-ray diffraction. The prepared catalysts were used to generate hydrogen gas through the water-splitting reaction under visible light (wavelengths greater than 400 nm). Various N/Ti addition ratios were tested, and the hydrogen generation rates were compared to determine the optimal ratio. The maximal hydrogen production rate (approximately 55 μmol h−1 g−1) was attained when the N/Ti ratio of N–TiO2 was 10. When PdO and Pt were loaded onto the N–TiO2 catalyst, the hydrogen generation rates increased to 544 and 772 μmol h−1 g−1, respectively. The highest hydrogen production rate (2460 μmol h−1 g−1) was obtained when bimetallic 0.05 wt% PdO-0.10 wt% Pt/N–TiO2 was used. After three times use the hydrogen yield of the catalyst was maintained as 83%. A possible mechanism of water splitting catalyzed by this visible light photocatalyst is proposed.  相似文献   

8.
Visible light active ABO3 type photocatalyst with LaFeO3 composition was synthesized by sol-gel method. The photocatalyst was characterized by different techniques such as X-ray diffraction, BET surface area analysis, particle size analysis, scanning electron microscopy, UV–visible diffuse reflectance spectroscopy (UV–Visible DRS), and photoluminescence spectroscopy. LaFeO3 photocatalyst exhibited an optical band gap of 2.07 eV with the absorption spectrum predominantly in visible region of the spectrum. The BET surface area of photocatalyst LaFeO3 was observed as 9.5 m2/g, with the crystallite size of 38.8 nm as calculated by the Debye-Scherer equation. The photocatalytic activity of LaFeO3 was investigated for hydrogen generation through sacrificial donor assisted photocatalytic water splitting reaction by varying conditions in feasible parametric changes using visible light source, ethanol as a sacrificial donor and Pt solution of H2PtCl6 as a co-catalyst. The rate of photocatalytic hydrogen evolution was observed to be 3315 μmol g−1 h−1 under optimized conditions and using 1 mg dose of photocatalyst with reaction time of 4 h and illumination of 400 W.  相似文献   

9.
In this study, we developed a polystyrene-platinum/nitrogen-doped titanium dioxide/strontium titanate composite-polyvinylpyrrolidone (PS-PNS-PVP) photocatalyst film, which is applied in the process of photocatalytic hydrolysis under simulated sunlight to produce hydrogen, is developed. PS, which is cheap, non-toxic, with high UV resistance, and chemical inertness, is used as a carrier, and a highly effective hydrogen production of Pt/N–TiO2/SrTiO3 as a photocatalyst. The influence of the PS concentration on the stability, optical, and electrical properties of the photocatalyst film is discussed. In addition, the influence of the photocatalyst dispersion in the film on the activity under various photocatalyst concentrations was investigated. A polyvinylpyrrolidone pore-forming agent was then used to examine the effect on the photocatalyst film structure and optical properties, and the subsequent influence on photocatalytic hydrogen energy activity. Adjusting the PS concentration to 20 wt% produced good film-forming stability, and the photocatalyst dispersibility in the film under different photocatalyst concentrations. A photocatalyst concentration of 2.5 wt% resulted in good film dispersibility and the realization of added pore-forming agent. The modified photocatalyst film changed the film from a blind pore structure to a connecting void structure, increasing the film's porosity and hydrophilicity. This increased the number of photocatalytic sites, and the optimal hydrogen production of the photocatalyst film reached 21,333 μmol h?1 g?1.  相似文献   

10.
Gold nanoparticles were deposited on potassium titanoniobate, KTiNbO5 using deposition-precipitation (DP), conventional impregnation (IMP) and photodeposition method in order to improve photocatalytic hydrogen production from water splitting. The effect of synthesis pH value of a HAuCl4 aqueous solution used in the DP process on the morphology of gold nanoparticles, optical property and photocatalytic activity of water splitting under UV light irradiation was investigated. These catalysts were characterized by powder X-ray diffraction patterns (XRD), inductively coupled plasma mass spectrometry (ICP-MS), UV–visible spectroscopy (UV–vis), and Transmission Electron Microscopy (TEM). The Au/KTiNbO5 catalysts prepared by the DP method consisted of a good metal–semiconductor interface which allowed for a much higher efficient electron-hole separation. The 0.63 wt% Au/KTiNbO5 catalyst prepared by the DP method at pH = 10 showed a uniform dispersion of gold nanoparticles with an average gold particle size of 4.2 nm and exhibited an ultra-high photocatalytic water splitting activity (3522 μmol g−1 h−1), about 47 times higher than that exhibited by the KTiNbO5 photocatalyst.  相似文献   

11.
A TiO2 nanotube-based nanoreactor was designed and fabricated by facile two steps synthesis: firstly, hydrothermal synthesized SrTiO3 was deposited on TiO2 nanotubes (TiO2NTs). Secondly, the Au nanoparticles (NPs) were encapsulated inside the TiO2NTs followed by vacuum-assisted impregnation. The as-synthesized composites were characterized using Transmission electron microscopy (TEM), X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Photoluminescence spectra (PL) and Ultraviolet–visible absorption spectroscopy (UV–vis). The photocatalytic performance was evaluated by the hydrogen evolution reaction. The results revealed that the SrTiO3 modified TiO2NTs confined Au NPs (STO-TiO2NTs@Au) achieved an enhanced hydrogen evolution rate at 7200 μmol h−1 g−1, which was 2.2 times higher than that of bald TiO2NTs@Au at 3300 μmol h−1 g−1. The improved photocatalytic activity could be attributed to the synergistic effect of the electron-donating of SrTiO3 and TiO2NTs confinement. The as-designed nanoreactor structure provides an example of efficient carriers' separation photocatalyst.  相似文献   

12.
In this paper, Pt3Ni alloy polyhedral was synthesized through solvothermal method and loaded on the surface of CdS by photo-induced electrons. Under visible light irradiation, the photocatalytic activity for hydrogen evolution from solar water splitting was performed, Pt3Ni/CdS showed the hydrogen evolution rate about 40.0 mmol/h/g (QE = 44.90%, λ = 420 nm), which was 1.8 times higher than that of Pt/CdS, indicating that Pt3Ni NPs could effectively improve the hydrogen production activity of CdS. Next, the influence of de-alloyed Pt3Ni NPs on the activity of CdS for water-splitting under visible light was investigated, the hydrogen evolution rate of de-alloyed Pt3Ni NPs modified CdS was 46.1 mmol/h/g (QE = 52.70%, λ = 420 nm), which was 1.2 times as much as that of Pt3Ni/CdS and 2.1 times as much as that of Pt/CdS, suggesting that de-alloyed Pt3Ni NPs could further enhance the hydrogen production activity of CdS. In addition, the improved photocatalytic activity was mainly due to the surface unsaturation of Pt atoms in a metastable structure after de-alloying, which will expose more surface active sites of Pt, thus the fast electron hole charge transfer at the interface of CdS and de-alloyed Pt3Ni NPs.  相似文献   

13.
La doped Cd2TaGaO6 photocatalyst was successfully synthesized for the first time by a sol–gel method. Several metal oxides and noble metals involving NiO, CuO, Cr2O3, Pt, and Ru were respectively loaded onto La doped Cd2TaGaO6 as cocatalyst. NiO and noble metal co-loaded photocatalyst was also prepared. The obtained products were characterized by X-ray diffraction (XRD), ultraviolet–visible spectra (UV–Vis), scanning electron microscope (SEM), etc. The results showed that most of cocatalyst loaded photocatalysts exhibited much higher activities for hydrogen evolution from ethanol aqueous solution than single La doped Cd2TaGaO6. Compared with sole NiO or noble metal loaded photocatalyst, NiO and noble metal co-loaded La doped Cd2TaGaO6 showed superior activity. It is revealed that the loaded NiO and noble metal can interact with each other and cooperate on improving the photocatalytic activity. The effect of the cocatalyst loading amount on photocatalytic properties was discussed. Especially, 0.5 wt% NiO and 0.5 wt% Pt co-loaded La doped Cd2TaGaO6 displayed the highest hydrogen production rate of 2.93 mmol h−1, which was ca. 33 times that of single La doped Cd2TaGaO6.  相似文献   

14.
Sensitized photocatalytic production of hydrogen from water splitting is investigated under visible light irradiation over mesoporous-assembled titanium dioxide (TiO2) nanocrystal photocatalysts, without and with Pt loading. The photocatalysts are synthesized by a sol–gel process with the aid of a structure-directing surfactant and are characterized by N2 adsorption–desorption analysis, X-ray diffraction, UV–vis spectroscopy, scanning electron microscopy, transmission electron microscopy and energy-dispersive X-ray analysis. The dependence of hydrogen production on the type of TiO2 photocatalyst (synthesized mesoporous-assembled and commercial non-mesoporous-assembled TiO2 without and with Pt loading), the calcination temperature of the synthesized photocatalyst, the sensitizer (Eosin Y) concentration, the electron donor (diethanolamine) concentration, the photocatalyst dosage and the initial solution pH is systematically studied. The results show that in the presence of the Eosin Y sensitizer, the Pt-loaded mesoporous-assembled TiO2 synthesized by a single-step sol–gel process and calcined at 500 °C exhibits the highest photocatalytic activity for hydrogen production from a 30 vol.% diethanolamine aqueous solution with dissolved 2 mM Eosin Y. Moreover, the optimum photocatalyst dosage and initial solution pH for the maximum photocatalytic activity for hydrogen production are 3.33 g dm−3 and 11.5, respectively.  相似文献   

15.
Chemically reduced graphene oxide (RGO) can be functionalized by eosin Y (EY). The formation of the stable aqueous EY functionalized graphene (EY-RGO) suspension is due to the non-covalent interaction between EY and RGO surface via hydrogen bonding and π-π stacking. EY-RGO was characterized by transmission electron microscopy (TEM), atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. Spectral and photoelectrochemical studies indicate that photoinduced electron transfer occurs from EY to RGO. The EY-RGO is photocatalytic active for water reduction to produce hydrogen. The average production rate of H2 for the photocatalyst (wEY/wRGO = 1) in a 10 vol% triethanolamine aqueous solution can reach 3.35 mmol g−1 h−1 and 0.40 mmol g−1 h−1 under 30 h UV-vis and 10 h visible light irradiation, respectively. The photocatalytic activity of EY-RGO is superior to that of RGO, graphene oxide (GO), and EY-GO. Modification EY-RGO with Pt nanoparticles can further improve photocatalytic activity. All these features demonstrated that organic sensitizers functionalized graphene provided a nice candidate as a photocatalyst for H2 generation from water under solar light irradiation.  相似文献   

16.
Tri-doped photocatalyst, SrTiO3:Ni/Ta/La, was prepared by spray pyrolysis from aqueous and polymeric precursor solutions. The third dopant, La3+, contributed to the BET surface area and porous morphology by preventing crystal growth, and increased the Ni2+/Ni3+ ratio by affecting the electron configuration in the lattice structure, which is closely related to the hydrogen evolution rate. The hydrogen evolution rate of the tri-doped photocatalyst, SrTiO3:Ni(0.2 mol%)/Ta(0.4 mol%)/La(0.3 mol%), was increased by about 60%–895.2 μmol g−1 h−1 from the value of 561.2 μmol g−1 h−1 for the co-doped photocatalyst, SrTiO3:Ni(0.2 mol%)/Ta(0.4 mol%), and was further enhanced to 2305.7 μmol g−1 h−1 when a polymeric precursor was used instead of an aqueous precursor in spray pyrolysis. The optimum additive content for polymeric precursor solution was 300 mol%.  相似文献   

17.
(AgNbO3)1−x(SrTiO3)x samples were successfully employed as photocatalysts for photocatalytic hydrogen evolution under visible light. The samples were characterized by a series of techniques, including X-ray diffractometry, scanning electron microscopy, UV–Vis spectrophotometry, and electrochemistry technology. The band gaps of (AgNbO3)1−x(SrTiO3)x solid solutions can be tuned continuously from 3.21 to 2.65 eV and the flat-band potentials (Vfb) can be shifted positively from −0.79 to −0.31 V vs. SHE when x decreased from 1 to 0. Band positions of (AgNbO3)1−x(SrTiO3)x samples were further testified by density functional theory, suggesting that the band gap narrowing of the solid solutions derived from the hybridization of (Ti 3d and Nb 4d) and (O 2p and Ag 4d) orbital. The photocatalytic activities of samples for H2 evolution with Pt cocatalyst were evaluated in aqueous methanol solution under visible light irradiation. The highest photocatalytic activity was obtained at (AgNbO3)0.25(SrTiO3)0.75. Photocatalytic activity in hydrogen evolution of these solid solutions proved to be closely dependent on band structures.  相似文献   

18.
Solar-driven photocatalytic hydrogen generation by splitting water molecules requires an efficient visible light active photocatalyst. This work reports an improved hydrogen evolution activity of visible light active TiO2-x photocatalyst by introducing reduced graphene oxide via an eco-friendly and cost-effective hydrothermal method. This process facilitates graphene oxide reduction and incorporates intrinsic defects in TiO2 lattice at a one-pot reaction process. The characteristic studies reveal that RGO/TiO2-x nanocomposites were sufficiently durable and efficient for photocatalytic hydrogen generation under the visible light spectrum. The altered band gap of TiO2-x rationally promotes the visible light absorption, and the RGO sheets present in the composites suppresses the electron-hole recombination, which accelerates the charge transfer. Hence, the noble metal-free RGO/TiO2-x photocatalyst exhibited hydrogen production with a rate of 13.6 mmol h?1g?1cat. under solar illumination. The appreciable photocatalytic hydrogen generation activity of 947.2 μmol h?1g?1cat with 117 μAcm?2 photocurrent density was observed under visible light (>450 nm).  相似文献   

19.
Rutile TiO2 nanosheets were prepared by a simple solvothermal process, and Cu was loaded on the surface of TiO2 nanosheets using the in situ photo-deposition method. Meanwhile, photocatalytic H2 evolution from water over the as-prepared TiO2 nanosheets loaded with Cu was explored using methanol as a sacrificial reagent. The results indicate that the TiO2 nanosheets loaded with Cu is an efficient photocatalyst under UV irradiation. During the first 5 h, a rate of H2 evolution of approximately 22.1 mmol g−1 h−1 was achieved under optimal conditions. Furthermore, for practical purposes, the photocatalytic hydrogen evolution was studied as a function of content of Cu, pH of solution, concentration of methanol and dosage of photocatalyst, respectively. At last, the photocatalytic mechanism was preliminarily discussed.  相似文献   

20.
Effect of photodeposition of AuNPs (gold nanoparticles) on TiO2, CeO2, Cu2O and Fe3O4 supports has been illustrated on sacrificial donor based hydrogen evolution. The synthesized samples were characterized by diffuse reflectance spectroscopy (DRS), and transmission electron microscopy (TEM). Highest photocatalytic activity was exhibited by Au/TiO2 followed by Au/Fe3O4, Au/CeO2 and Au/Cu2O. Au/TiO2 under optimized conditions has shown significantly high photocatalytic activity under both UV–visible and visible radiation. Au/TiO2 shows hydrogen evolution rate of 920 μmol h−1 and 32.4 μmol h−1 under UV–visible and visible radiation, respectively. Significant enhancement in hydrogen evolution rate under visible light is very encouraging and may be attributed to polydispersed nature of AuNPs wherein larger particles facilitate light absorption and the smaller function as catalytic sites. Further studies are in progress to study the influence of various parameters on photocatalytic activity of Au/TiO2.  相似文献   

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