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1.
The use of floatable photocatalyst supports is an operable strategy of increasing photocatalytic performance in terms of improving light absorption. In this work, floatable organic support based on poly(vinyl alcohol) (PVA) was used to float commercial TiO2 P25 nanoparticles. At first, by the use of CaCl2 and boric acid at pH 3 the cross-linking of PVA blended with sodium alginate (PVA-Alg) was improved to enhance chemical and mechanical stability, and then it was chemically modified by trimethylchlorosilane to achieve floatable organic support (modified or MPVA-Alg). The prepared support and photocatalyst were characterized by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy, energy-dispersive X-ray spectroscopy (EDX)-elemental mapping, inductively coupled plasma optical emission spectroscopy, ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy, photoluminescence (PL), thermalgravimetry, Brunauer-Emmett-Teller (BET), and water contact angle (WCA) analyses and applied for the ammonia degradation under UV to visible regions. Results of WCA and FTIR confirmed that chemical modification of PVA-Alg led to lowering hydrophilicity to be floated on the ammonia wastewater. UV-vis analysis indicated that the MPVA-Alg acts as a light absorbent in UV-vis ranges and makes TiO2/MPVA-Alg a visible light active composite. Also, the PL analysis showed that the charge recombination process was strongly suppressed in the case of the TiO2/MPVA-Alg sample. BET theory suggested that the textural properties were not the key factor in determining photocatalytic performance. The maximum photocatalytic ammonia removal was obtained to be 63% and 57% by the TiO2/MPVA-Alg composite under UV-vis light irradiations, respectively. The MPVA-Alg and TiO2 exhibited the ammonia degradation of 28.5% and 15.2% under visible and 29.4% and 40.0% under UV irradiation, respectively. The TiO2/MPVA-Alg showed favorable reuse ability after five runs due to desirable chemical and mechanical resistance. This study provides an insight into the modification of polymeric structures to be used as both floatable photocatalyst support and light sensitizer.  相似文献   

2.
The application of hydrogen energy potentially addresses energy and environmental problems. In order to improve the photocatalytic efficiency, nanocomposite of N-doped TiO2 with graphene oxide (NTG) is prepared and characterized with Fourier transform infrared spectra (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectra, X-ray photoelectron spectroscopy (XPS), atomic force microscope (AFM), photoluminescent spectra. The application of NTG to hydrogen evolution exhibits high photocatalytic efficiency of 716.0 or 112.0 μmol h−1 g−1 under high-pressure Hg or Xenon lamp, which is about 9.2 or 13.6 times higher than P25 photocatalyst. This is mainly attributed to the N-doping of TiO2 and the incorporation of graphene oxide resulting in narrow band gap, together with the synergistic effect of fast electron-transporting of photogenerated electrons and the efficient electron-collecting of graphene oxide retarding charge recombination. These results provide a significant theoretical foundation for the potential application of N-doping photocatalysts to hydrogen evolution.  相似文献   

3.
Abstract

Abstract

Thin films of anatase TiO2 nanotube arrays (TiO2 NTs) were prepared in this study. Pt and Ag were coated on the TiO2 NTs films, which intend to increase the photocatalytic activity under ultraviolet-visible (UV-vis) irradiation. The phase and structure of the films were investigated by X-ray diffraction and scanning electron microscopy. Photocatalytic activity was tested by UV-vis absorption spectroscopy and showed that UV-vis light absorption of the films was remarkably improved by coated Ag and Pt by 72% and 183% respectively. The photocatalytic activities of the films towards degraded methyl orange and HCHO were compared and were all found to follow the sequence Pt/TiO2 NTs>Ag/TiO2 NTs>TiO2 NTs. It was also found that the kinetics of HCHO photocatalytic degradation by the films fits the first order reaction model better and has higher efficiency than that of the methyl orange photocatalytic degradation by the same films.  相似文献   

4.
AuPd bimetallic nanoparticle (NP) modified ultra-thin graphitic carbon nitride nanosheet photocatalysts were synthesized via photochemical deposition-precipitation followed by hydrogen reduction. The crystal structure, chemical properties, and charge carrier behavior of these photocatalysts were characterized by X-ray diffraction (XRD), surface photovoltage spectroscopy (SPS), transient photovoltage spectroscopy (TPV), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), and UV-Vis diffuse-reflectance spectroscopy (DRS). Photocatalytic H2 evolution experiments indicate that the hydrogen treated AuPd nanoparticles can effectively promote the separation efficiency of electron-hole pairs photo-excited in the g-C3N4 photocatalyst, which consequently promotes photocatalytic H2 evolution. The 1.0 wt% AuPd/g-C3N4 (H2) composite photocatalyst showed the best performance with a corresponding photocatalytic H2 evolution rate of 107 μmol h?1. The photocatalyst can maintain most of its photocatalytic activity after four photocatalytic experiment cycles. These results demonstrate that the synergistic effect of light reduction and hydrogen reduction of AuPd and g-C3N4 help to greatly improve the photocatalytic activity of the composite photocatalyst.  相似文献   

5.
The development of excellent photocatalytic material is highly required for energy and environmental applications. In this study, visible light responsive p-n heterojunction photocatalysts based on CuO/MoO3 with varying ratios of CuO were prepared by the facile hydrothermal method. The crystalline structure, surface morphology, chemical compositions and optical properties of the synthesized photocatalysts were studied using X-ray powder diffraction (XRD), scanning electron microscopy (SEM), Energy-dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared spectroscopy (FTIR), photoluminescence (PL) techniques and UV–Vi's absorption spectroscopy. The results showed that the 5%CuO/MoO3 nanocomposite displayed enhanced photocatalytic performance for the production of hydrogen (98.5 μmol h?1g?1) and degradation of dyes rhodamine B (RhB) and alizarine yellow (AY) than all other samples. Furthermore, 5% CuO/MoO3 composite exhibited excellent stability after five consecutive cycles for both RhB and AY dyes. Overall, the improved photocatalytic performance of 5%CuO/MoO3 composite was due to increased adsorption of visible light, good surface morphology, enhanced charge separation/transfer which inhibited recombination of electrons and holes. This study could encourage the synthesis of novel and effective p-n heterojunction photocatalysts for practical applications.  相似文献   

6.
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   

7.
Developing efficient, stable, and cheap photocatalysts for H2 production has aroused great interest among researchers. Herein, noble-metal-free ZnO/SrTiO3 composite photocatalysts have been successfully prepared by hydrothermal method. X-ray diffraction, field-emission scanning electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, ultraviolet–visible diffusion spectroscopy, and photoluminescence spectroscopy are used to characterize the obtained samples. The photocatalytic water splitting for H2 production by ZnO/SrTiO3 has been studied under simulated sunlight irradiation by using triethanolamine as a sacrificial agent and Eosin Y (EY) dye as a sensitizer. The orthogonal experiments are designed to optimize the photocatalytic reaction conditions for practical purposes. The influencing extents and trends of the factors have been investigated, including the catalyst composition and dosage, pH value of the solution, triethanolamine, and EY addition. Under the optimum conditions, the H2 production rate with ZnO/SrTiO3 is up to 16006.12 μmol g?1 h?1. The excellent performance of ZnO/SrTiO3 is attributed to the formation of a step-scheme (S-scheme) heterojunction, which promotes the separation of photocarriers and reduces their recombination probability.  相似文献   

8.
We present a simple two-step hydrothermal method to prepare AgInZnS/MoS2 nanocomposite. The morphology and compositional characteristics of the sample were investigated by field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The as-synthesized heterostructures exhibited superior photocatalytic activity for hydrogen evolution under visible-light irradiation and the optimum loading amount of MoS2 is at 0.5 wt%. In an attempt to explain this phenomenon, a possible mechanism was also proposed. The enhanced photocatalytic activities toward water splitting arise from the boosted active sites for hydrogen generation and the enhanced charge transfer. This work may contribute to the design and construction of highly efficient visible-light responsive photocatalyst for sustainable energy harvesting and conversion.  相似文献   

9.
Seeking an efficient and non-precious co-catalyst for g-C3N4 (CN) remains a great demanding to achieve high photocatalytic hydrogen generation performance. Herein, a composite photocatalyst with high efficiency was prepared by modifying CN with coral-like NiSe2. The optimal hydrogen evolution rate of 643.16 μmol g?1 h?1 is from NiSe2/CN-5 under visible light. Superior light absorption and interfacial charge transfer properties including suppressed photogenerated carrier recombination and efficient separation of photogenerated electron-hole pairs have been observed, which account for the enhanced photocatalytic performance of CN.  相似文献   

10.
N-doped TiO2 nanoparticles were prepared by using 1° and 2° alkyl and alcohol amines [n-propylamine (nPRYL), ethanolamine (ETOH), propanolamine (PROH), diethylamine (DETYL), dipropylamine (DPRYL), diethanolamine (DETOH), and ammonium hydroxide (NH4OH)] as nitrogen sources through microwave and hydrothermal growth (HT) methods. Characterization of the nanoparticles was done by X-ray diffraction, scanning electron microscopy, ultraviolet-visible absorption spectra, X-ray photoelectron spectroscopy, fourier transform infrared spectroscopy and BET analysis techniques. Nitrogen species in TiO2 lattice were interstitial impurities. Nitrogen content of the particles depended on the preparation conditions and structural differences of nitrogen sources. Photocatalytic degradation of methylene blue was carried out under Xenon lamp irradiation. N-doped TiO2 nanoparticles exhibited higher photocatalytic activity, compared to undoped ones. Acidity differences of amine sources and irradiation differences of synthetic conditions had an effect on photocatalytic activity. Although N doping into TiO2 lattice was the least effective in the particle prepared by the use of nPRYL as the amine source and HT as the synthetic condition, its photocatalytic activity was slightly better compared to others.  相似文献   

11.
Cobalt oxide (Co3O4) nanoparticles decorated on mesoporous carbon nitride (Co3O4/MCN) nanocomposites for photocatalytic hydrogen evolution were investigated in this work. MCN was prepared using 3-amino-1,2,4-triazole, high nitrogen content, as a single molecular carbon and nitrogen precursor and SiO2 nanoparticles as the hard template. Complementary characterization techniques were employed to understand the textural and chemical properties of the nanocomposites. The bare MCN showed high photocatalytic activity under visible light irradiation without using any co-catalyst. The photocatalytic activity of Co3O4/MCN with a Co3O4 mass content of 5 wt % presented two times higher than the bare MCN, which is attributed to the enhanced visible-light harvesting and more efficient charge separation. Mechanistic study shows lower electron-hole recombination rate, higher charge separation efficiency occurs after the formation of p-n type heterojunction.  相似文献   

12.
Visible-light-induced heterostructure photocatalysts have been regarded as promising candidates in clean energy production and environmental treatment of organic pollutants. In this study, we have prepared nanocomposites of V2O5/N-deficient g-C3N4 (VO/Ndef-CN), which have been characterized by a variety of techniques. The as-synthesized nanocomposites show efficient bifunctional photocatalytic properties toward hydrogen generation and pollutants degradation (dye and antibiotic). The optimized 5VO/Ndef-CN photocatalyst exhibits improved photoactivity for H2 production (5892 μmol g?1 h?1), with a high quantum yield of 6.5%, and fast degradation of organic pollutants, as well as high photocatalytic stability under visible light irradiation. The high photocatalytic efficiency is due to the presence of N defects and S-scheme heterojunction formation, which leads to rapid charge separation, enhanced visible-light absorption, and increased active sites. Furthermore, the possible activity-enhanced mechanism and the photodegradation pathway are proposed based on the experimental and density functional theory (DFT) investigations.  相似文献   

13.
In the present work, physical, photo-electrochemical properties and photocatalytic activity of Cu(Cr1-x,Alx)2O4 (x = 0, 0.1, 0.5, 0.9 and 1) spinels synthesized via the nitrate route were investigated for the first time. X-ray diffraction (XRD) with Rietveld refinement confirms the purity of all samples while SEM images show the porous and spongious morphology of the oxides of 62–311 nm grain sizes. The chemical composition and the oxidation states were determined by X-ray photoelectron spectroscopy (XPS) analysis. The specific surface area is highly affected by x-ratio. The photoelectrochemical behavior of the synthesized materials was evaluated by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and Mott-Schottky in Na2SO4 electrolyte (0.1 M). Indeed, the electrochemical tests under the effect of light show an increase in the current intensity and a decrease in the charge transfer resistance in CV and EIS tests, respectively. These materials were applied as photocatalysts for the photodegradation of Methylene Blue (MB) under UV light with the aid of H2O2 serving as generator of free radicals. Our results show that Cu(Cr0.1,Al0.9)2O4 is the most performant photocatalyst of MB with a degradation efficiency of 98.8% within 80 min of irradiation. Furthermore, the photocatalytic activities of Cu(Cr0.1,Al0.9)2O4 were evaluated by the degradation of Rhodamine B (RhB) and Methyl Orange (MO) and the results reveal a good performance toward RhB degradation (85.5%), and to a lesser degree for MO decomposition (67.3%).  相似文献   

14.
Considering the renewability and cleanness of hydrogen generation system, the photocatalytic H2 evolution through water splitting with assistance of Earth abundant co-catalysts has become a scientific hotspot. Efficient and visible light driven CdO-WO3 composites with versatile properties have been fabricated through hydrothermal approach for H2 evolution. X-ray diffractometer, scanning electron microscope, UV-Vis absorption spectroscopy, photoluminescence emission spectroscopy and photocatalytic activity test were employed to investigate different properties like crystallography, morphology, optical and photocatalytic properties. The effect of CdO concentration on the grain size indicated the reduction of bad gap energy of the WO3. The concentration of CdO nanoparticles in WO3 directly effect on the morphology of the particles that are in the form of nanorods. The atoms of CdO makes the WO3 nanoparticles more effective and efficient up to 4% of CdO but when coupling amount increases then the CdO-WO3 nanoparticles exhibited less photocatalytic performance to evolve H2 energy. Results shown that 4% content in WO3 had exceptional photocatalytic activity for water splitting when compared to other samples. The improved hydrogen production was allied with formation of active Cd species during the photocatalysis process, which has the ability to promote the interfacial charge-separation and concurrently may cause to reduce the over potential of hydrogen evolution, thus boosting the photocatalytic activity over the hybrid sample. The improved photocatalytic activity of composites could be accredited to extended absorption region of visible light, efficient separation of charge carrier's and suppress recombination of electron-hole pairs. The current work not only shows a prospect for the utilization of low cost CdO as a co-catalyst in photocatalytic hydrogen generation but also shows a substantial enhancement in H2 evolution, first time, using CdO-WO3 hybrid photocatalyst.  相似文献   

15.
In this study, the optimization of hydrogen production by photocatalytic steam methane reforming over Lanthanum modified TiO2 has been investigated using response surface methodology. The La/TiO2 photocatalysts were synthesized using wet impregnation method and characterized for physicochemical and photocatalytic properties by N2 physisorption, X-ray powder diffraction (XRD), Scanning electron microscopy (SEM), Energy dispersive X-ray (EDX), and ultraviolet-visible (UV-vis) spectroscopy. The characterization shows that the La/TiO2 possesses appropriate properties to be used as photocatalysts. The photocatalysts were employed in the optimization studies of hydrogen production by photocatalytic steam methane reforming. The effects of irradiation time (10–150 min), metal loading (1–3%), methane concentration (10–50%), and steam concentration (0.5–1.5%) on the rate of hydrogen production were determined employing Box-Behnken experimental design. The application of the RSM resulted in the formulation of four models out which the quadratic model was adjudged to adequately fit the experimental data. A further statistical analysis of the quadratic model established the significance of the model with p-value far less than 0.05 and coefficient of determination (R2) of 0.975. A non-significant lack of fit obtained for the model further confirm the suitability of the quadratic model in fitting the experimental data. At the desirability function of 1, optimum conditions of 146.15 min, 2.94%, 22.83% and 1.24% for irradiation time, metal loading, methane concentration, and steam concentration, respectively resulted in the production of 2.42 μmol of hydrogen/min.  相似文献   

16.
In this article, a ternary WO3/g‐C3N4@ BiVO4 composites were prepared using eco‐friendly hydrothermal method to produce efficient hydrogen energy through water in the presence of sacrificial agents. The prepared samples were characterized by scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM), transmission electron microscopy (TEM), X‐ray diffraction (XRD), ultraviolet‐visible (UV‐vis), Brunauer‐Emmett‐Teller (BET) surface area, and photoluminescence spectroscopy (PL) emission spectroscopy. The experimental study envisages the formation of 2‐D nanostructures and observed that such kinds of nanostructures could provide more active sites for photocatalytic reduction of water and their inherent reactive‐species mechanism. The results showed the excellent photocatalytic performance (432 μmol h?1 g?1) for 1.5% BiVO4 nanoparticles in WO3/g‐C3N4 composite when compared with pure WO3 and BiVO4. The optical properties and photocatalytic activity measurement confirmed that BiVO4 nanoparticles in WO3/g‐C3N4 photocatalyst inhibited the recombination of photogenerated electron and holes and enhanced the reduction reactions for H2 production. The enhanced photocatalytic efficiency of the composite nanostructures may be attributed to wide absorption region of visible light, large surface area, and efficient separation of electrons/holes pairs owing to synergistic effects between BiVO4 and WO3/g‐C3N4. The prepared samples would be a precise optimal photocatalyst to increase their suppliers for worldwide applications especially in energy harvesting.  相似文献   

17.
For better utilization of solar spectrum and complete redox of water for water splitting applications, it is required to have a semiconductor which is photoactive in visible region. In this study, we report theoretical and experimental investigations on morphological and opto-electronic modifications induced in α-Bi2O3 due to Selenium (Se) doping tested for photoelectrochemical (PEC) & photocatalytic properties. Density Functional Theory (DFT) calculations revealed band gap reduction and direct to indirect transitions in Se-doped α-Bi2O3. This reduction in band gap is attributed to hybridization of Se p & Bi s in valence band and Se d & Bi p orbital in conduction band. To support this finding experimentally, we synthesized Se-doped α-Bi2O3 using simple chemical precipitation method and measured its band gap using photoluminescence and UV–Vis spectroscopy. Experimental results also confirmed the reduction in band gap energy and recombination rate of charge carriers as compared to pristine α-Bi2O3 sample. PEC study of Se-doped α-Bi2O3 showed an increased photocurrent density, charge carrier density and lowered impedance, which indicates its efficient solar spectrum utilization and better hydrogen generation efficiency. Photocatalytic measurement also revealed higher rate of dye degradation with Se doped α-Bi2O3.  相似文献   

18.
The nanocomposite material C@Pt/MoS2@CdS was prepared by a simple microwave-assisted hydrothermal method combined with photoreduction method. The crystal structure, microstructure, and surface physical chemistry properties of the material were analyzed by X-ray diffraction (XRD), ultraviolet–visible diffuse reflectance absorption spectroscopy (UV–vis/DRS), X-ray photoelectron energy spectroscopy (XPS), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HR-TEM), nitrogen adsorption–desorption measurement, photoluminescence spectroscopy (PL), and electrochemical tests. As a result, this material has full-spectrum light absorption property and the composited CdS presents a good hexagonal phase. Moreover, the composite material presents a nanorod-like multi-layer core-shell structure, wherein the rod-like MoS2@CdS surface is covered with Pt and C. The formation of the multi-layer core-shell structure increases the specific surface area of as-composite material and strengthens its light absorption performance. The electrochemical impedance and transient photocurrent test results show that C@Pt/MoS2@CdS has the highest charge separation efficiency and enhanced photocurrent density compared with other systems. Photogenerated charge carriers have higher separation efficiency, and photogenerated electrons and holes exhibit longer life. During the photocatalysis experiments, the nanocomposite C@Pt/MoS2@CdS shows enhanced photodegradation activity under multi-modal photocatalytic experiments and excellent stability under visible light irradiation. In addition, C@Pt/MoS2@CdS has a strong photocatalytic water splitting ability. Under the same experimental conditions, its hydrogen production is 60 times that of commercially available P25. Through capture experiments, the reactive species in the photocatalytic reaction process were determined, and the possible photocatalytic reaction mechanism of this multi-layer core-shell C@Pt/MoS2@CdS nanocomposite was inferred.  相似文献   

19.
The photocatalytic activity for H2 evolution from pure water over Pd loaded TiO2 prepared by gardenia extract (Pd-Gardenia-TiO2) is systematically investigated. The as-prepared photocatalysts are characterized by X-ray diffraction, high resolution transmission electron microscopy, Fourier transform infrared spectra, and X-ray photoelectron spectroscopy. Gardenia extract functions as reducing and stabilizing agents simultaneously. The mean size of the as-prepared Pd nanoparticles is in the range of 2.3 ± 0.5 nm based on TEM images. The Pd-Gardenia-TiO2 catalyst exhibits good photocatalytic activity for H2 evolution (93 μmol · h−1 · g−1), which is much higher than that of Pd photodeposited on TiO2. Possible factors for its photocatalytic activity from pure water are also investigated.  相似文献   

20.
In this study, we describe the successful fabrication of CdS in ionic hydrogels by an in situ growth method and demonstrate that the as-prepared CdS in hydrogels (CdS/HGel) can be used as cost-effective and recyclable catalysts for photocatalytic hydrogen generation. The structure and morphology of CdS/HGels were characterized by various techniques including X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, UV-vis diffuse reflectance spectroscopy, and Fourier transform infrared spectroscopy. The resultant CdS in cationic hydrogel (CdS/HGelPDAM2) showed the best performance of photocatalytic hydrogen production and the hydrogen production rate was up to 10.35 or 7.70 mmol h−1 g−1 when triethanolamine or Na2S–Na2SO3 was used as sacrificial agent. However, CdS in anionic hydrogel (CdS/HGelPAAM) showed poor photocatalytic hydrogen production performance under the same conditions. The solution pH and sacrificial agent type are also indispensable factors that affect the photocatalytic hydrogen production. The enhancement of hydrogen production comes from interaction between polymer chains and Cd2+, high dispersibility of CaS nanoparticles in hydrogels, high hydrophilic and swelling ability of hydrogel, high diffusion rate of reactant in hydrogel, and inhibited binding possibility of photogenerated electron-hole pairs. Since CdS/HGelPDAM has excellent hydrogen production efficiency and ease recovery property, it will be a potential photocatalyst for photocatalytic reactions.  相似文献   

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