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1.
With the development of research on the photocatalytic water splitting and hydrogen (H2) precipitation, cobalt ferrite and molybdate have begun to appear as catalysts for the study of photocatalytic hydrogen precipitation. In this paper, the p-n heterojunction CoFe2O4/NiMoO4 (CFO/NMO) is prepared by hydrothermal method. The constructed p-n type (type Ⅱ) heterojunction CFO/NMO has the highest hydrogen evolution (Eosin Y as a sensitizer), which is 7.39 times and 1.95 times that of elemental CFO and NMO, respectively. After the CFO and NMO form a heterojunction, a built-in electric field is formed inside to effectively separate the photogenerated carriers. At the same time, the dense interface of the heterojunction also promotes the transfer of photogenerated carriers and promotes the reduction of H+ protons on this catalyst surface. In short, this work provides more possibilities for the field of photocatalytic hydrogen evolution from molybdate and cobalt ferrite compounds.  相似文献   

2.
Promoting the separation of electron and hole plays an important role in photocatalytic hydrogen production. However, single semiconductor materials cannot fully realize their potential due to the rapid recombination of photogenerated carriers. Therefore, in this experiment, a new photocatalyst ZnIn2S4/NiMoO4 was prepared by using an electrostatic self-assembly method, which greatly improved the electron-hole recombination phenomenon. After 5 h reaction under visible light irradiation, ZIS/NMO-3 composite catalyst prepared in ethanol showed the best photocatalytic activity, and the hydrogen evolution capacity reached 173.09 μmol. The hydrogen evolution capacity of ZIS/NMO-3 was 2.47 and 25.83 times that of short rod-like NiMoO4 and microflower-like spherical ZnIn2S4, respectively. Through some physical characterization and electrochemical experiments, it can be seen that NiMoO4 and ZnIn2S4 have good composability. Meanwhile, the composite catalyst ZnIn2S4/NiMoO4-3 has high current response characteristics. It can be seen from the fluorescence emission spectra that the composite catalyst presents the lowest peak value, which indicates that ZIS/NMO-3 can effectively inhibit the recombination of photogenerated electrons and holes. When ZnIn2S4 is loaded on NiMoO4, the separation of photogenerated carrier will be accelerated due to the formation of heterojunction, thus improving the photocatalytic activity. At the same time, the large specific surface area will also provide more abundant active sites for the composite catalyst, which provides a good condition for photocatalytic hydrogen production. This work provides an efficient, uncomplicated and feasible method for the synthesis of ZIS/NMO-3 composite catalyst with excellent properties.  相似文献   

3.
The heterojunction construction can effectively regulate the carrier transport pathway. Ag2Mo2O7/CoMoO4 composite molybdate material was successfully synthesized by one step hydrothermal calcination method. The preparation method makes the contact of the two molybdate salts closer, forming a stable S-scheme heterojunction. Then SnS2 was added under physical agitation to improve the mobility of photogenerated carriers. The excellent structure of the ternary composite catalyst was proved by morphology and element analysis. The electron transfer mechanism of the S-scheme heterojunction was studied by photoelectric chemical test and spectral analysis. Because of the successful construction of S-scheme heterojunction and the introduction of sensitizer SnS2, the composite catalyst showed excellent hydrogen evolution performance (1599 μmol·g−1·h−1). This is because the S-scheme heterojunction and the sensitizer cooperatively promote the electron accumulation at the conduction band of CoMoO4. This work will provide a new strategy for molybdate in a heterojunction construction scheme.  相似文献   

4.
In present study, photocatalytic production of alkanes and hydrogen gas from butyric acid solution over Cu2O/Bi2WO6 composites has been investigated under UV irradiation. The Cu2O/Bi2WO6 heterojunction composites were synthesized by a two-step method, first by a hydrothermal method, and then by a simple reduction precipitation method. The as-prepared samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), ultraviolet–visible diffuse reflection spectroscopy (DRS) and photoluminescence spectroscopy (PL). In Cu2O/Bi2WO6 composites, the larger spherical Cu2O were covered by smaller Bi2WO6 nanosheets. The 24.36 wt%Cu2O/Bi2WO6 composite showed the highest photocatalytic activity for production of alkanes and hydrogen gas. The enhancement in photocatalytic activity can be ascribed to increment in light absorption and effective inhibition of recombination of photogenerated carriers at the heterostructure interface. Based on distributions of gaseous products and intermediates in liquid, a possible mechanism for photocatalytic decomposition of butyric acid over Cu2O/Bi2WO6 composites is proposed. Our results provide a method for pollutants removal with simultaneous production of alkanes and hydrogen.  相似文献   

5.
In this work, Au was loaded on the ZnO–TiO2 heterojunction by the deposition-precipitation with urea method to boost its photocatalytic hydrogen production. The synthesized materials were characterized by TEM, ICP-OES, XRD, N2 adsorption-desorption, UV–vis spectrophotometry, XPS, and (photo)electrochemical measurements. The TEM images confirmed the close contact between ZnO and TiO2 nanoparticles and showed that although Au nanoparticles agglomerated in the form of islands; they were widely dispersed on the surface of the photocatalysts. Besides, the XPS characterization revealed the enhanced contribution by the metallic Au species as their amount was increased in the composite. The heterojunctions with different Au contents produced higher yield in the photocatalytic production of hydrogen, observing a maximum with the 2-wt.%- Au content (9.13 mmol g−1), being this value 6 times higher than the results obtained with the ZnO–TiO2 heterojunction. This improvement is associated with the synergistic interaction between the ZnO–TiO2 heterojunction and Au islands that promoted the separation and transfer of charge carriers. Besides, the (photo)electrochemical characterization showed that the islands acted as “electronic reservoirs”, prolonging the lifetime of the photogenerated electron-hole pairs and creating surface or energy states at the Au/ZnO–TiO2 heterojunction interface. These states helped improve the charge transfer processes by diminishing the recombination and increasing the photocatalytic hydrogen production.  相似文献   

6.
Direct Z-scheme Bi2WO6/TiO2 heterojunction photocatalyst was prepared by one-step solvothermal method. The catalyst was characterized by XRD, TEM, XPS, UV–Vis DRS, photoluminescence spectroscopy and photoelectrochemical studies. The photocatalytic hydrogen production experiments show that Bi2WO6 did not generate H2 and the H2-production rate of TiO2 is only 0.1 mmol⋅g−1h−1. The hydrogen production rate of the Bi2WO6/TiO2 heterojunction photocatalyst reaches 12.9 mmol⋅g−1h−1, which is 129 times that of TiO2. Compared with TiO2, the enhanced H2-production activity of the heterojunction catalyst can be attributed to the wider light absorption range and the efficient separation and migration of carriers at the close contact interface between Bi2WO6 and TiO2. Based on the work functions of Bi2WO6, TiO2 and their heterojunctions, combined with the results of electron paramagnetic resonance spectroscopy and Mott-Schottky measurements, the photocatalytic H2 production mechanism of Z-scheme heterojunction Bi2WO6/TiO2 was proposed. This work provides an easy and simple way to design a binary Z-scheme photocatalyst with efficient catalytic H2-production activity without electron mediators.  相似文献   

7.
Constructing 2D/2D heterojunction photocatalysts has attracted great attentions due to their inherent advantages such as larger interfacial contact areas, short transfer distance of charges and abundant reaction active sites. Herein, 2D/2D CoP/CdS heterojunctions were successfully fabricated and employed in photocatalytic H2 evolution using lactic acid as sacrificial reagents. The multiple characteristic techniques were adopted to investigate the crystalline phases, morphologies, optical properties and textual structures of heterojunctions. It was found that integrating 2D CoP nanosheets as cocatalysts with 2D CdS nanosheets by Co–S chemical bonds would significantly boost the photocatalytic H2 evolution performances, and the 7 wt% 2D/2D CoP/CdS heterojunction possessed the maximal H2 evolution rate of 92.54 mmol g?1 h?1, approximately 31 times higher than that of bare 2D CdS nanosheets. Photoelectrochemical, steady photoluminescence (PL) and time-resolved photoluminescence (TRPL) measurements indicated that there existed an effective charge separation and migration over 2D/2D CoP/CdS heterojunction, which then markedly lengthened the photoinduced electrons average lifetimes, retarded the recombination of charge carriers, and caused the dramatically boosted photocatalytic H2 evolution activity. Moreover, the density functional theory (DFT) calculation further corroborated that the efficient charge transfer occurred at the interfaces of CoP/CdS heterojunction. This present research puts forward a promising strategy to engineer the 2D/2D heterojunction photocatalysts endowed with an appealing photocatalytic H2 evolution performance.  相似文献   

8.
A high-efficiency and easy-available approach was developed to obtain a ternary heterojunction composites with advanced hydrogen evolution reaction (HER) performance under visible light by water split. PdAg bimetallic nanoparticles make a close contact interface between g-C3N4(CN) and Zn0.5Cd0.5S(ZCS). Under visible light irradiation, CN and ZCS are both excited to generate electron-hole pairs, PdAg bimetallic nanoparticles act as a bridge between CN and ZCS. Not only can the photogenerated electrons from CN be captured, but they can also be quickly transferred to the surface of ZCS and participate in the photocatalytic reaction to release H2, and the recombination of charge carriers between the contact interface of ZCS and CN can be significantly inhibited. In addition, the thin CN layer reduces the photocorrosion of the ZCS and enhances the specific surface area of the composite material. After testing, the composite material with 30 wt% ZCS and 4 wt% PdAg demonstrates hydrogen evolution performance, up to 6250.7 μmol g?1h?1, which is 753 times the hydrogen evolution rate of single-component CN and 12.6 times of ZCS/CN. Compared with single-component and two-component photocatalysts, the ternary ZCS/PdAg/CN photocatalyst achieves significantly enhanced photocatalytic activity.  相似文献   

9.
In this paper, a g-C3N4/WO3-carbon microsphere composite-based photocatalyst was successfully prepared by a one-pot thermal synthesis method for sunlight driven decomposition of water to produce hydrogen. The results show that the g-C3N4/WO3-carbon microspheres had better photocatalytic properties and stability. Under visible light and sunlight irradiation, the hydrogen production efficiency of the photocatalytic decomposition of water was 107.75 times and 70.54 times greater than that of pure g-C3N4, respectively. The experimental and characterization results show that g-C3N4 and WO3 formed a Z-scheme heterojunction on the surface of the g-C3N4/WO3-carbon microsphere composite-based photocatalyst. Carbon microspheres modified on g-C3N4 nanosheets and WO3 had good conductivity and promoted the transfer of photogenerated electrons in g-C3N4 nanosheets. The addition of carbon microspheres increased the specific surface area of the composite photocatalyst. The g-C3N4/WO3-carbon microsphere composite-based photocatalyst showed strong adaptability to the fluctuating light intensity, providing feasibility for industrialized mass production.  相似文献   

10.
Semiconductor photocatalysts can convert solar energy into clean pollution-free hydrogen energy and thus are a novel technology to alleviate the energy crisis. To acquire catalysts with higher photocatalytic hydrogen production efficiency, we synthesized ZnCdS catalysts from a hydrothermal method and the WO3 cocatalyst through temperature-programmed reduction. The surface morphology and optical properties of the catalysts were characterized via X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and UV–Vis spectroscopy, which proved the successful synthesis of the WO3/ZnCdS compound catalysts. The effects of WO3 dosage on the photocatalytic activity of ZnCdS were studied, and in particular, the hydrogen production activity of the 35 wt% WO3/ZnCdS was the highest to 98.68 μmol/mg, about 9.6 times that of pure ZnCdS (10.28 μmol/mg). After 5 cycles, it yet had high repeatability and preserved high hydrogen production activity after 100 h of photocatalytic tests. The underlying mechanism was explored via photoluminescence and photocurrent assays. It was found the 35 wt% WO3/ZnCdS generated higher photocurrent than pure ZnCdS, indicating WO3 could facilitate electron transfer to involve more electrons in hydrolysis reactions, thereby increasing the photoelectron use efficiency and photocatalytic hydrogen production activity.  相似文献   

11.
Free-standing carbon nanotube films (CNTF) with entangled carbon nanotubes (CNT) were used as conductive supports for the preparation of CuS–ZnS/CNTF composite as immobilized photocatalysts for H2 production. The surface morphology, crystalline property, surface chemistry, and optical properties of the CuS–ZnS/CNTF photocatalysts were investigated. The effects of forming CuS–ZnS heterojunction and conductive CNTF on the separation of photogenerated charges and photocatalytic hydrogen production activity of CuS–ZnS/CNTF photocatalysts were evaluated by the photocatalytic hydrogen production tests. Conductive CNT films can prevent the recombination of photogenerated electron–hole pairs. The deposition of CuS nanoparticles on the ZnS/CNTF leads to higher photocatalytic activity which can be attributed to the effective electron–hole separation. Introducing ZnS and CuS makes the photocatalyst surface more hydrophilic. The porous structure contributed to the effective contact between the sacrificing agents and the photocatalysts, leading to enhanced H2 production activity.  相似文献   

12.
Constructing direct Z-scheme heterostructure is an effective way to promote the separation of photogenerated carriers and optimize the redox ability of the photocatalytic system. This work reports the in-situ synthesis of sea-urchin-like ZnS/SnO2 Z-scheme heterojunctions via a one-step hydrothermal method. Both experimental results and density functional theory (DFT) calculations indicate that the tight interfaces derived from in-situ precursor dissociation can ensure a fast transfer for photogenerated carriers, meanwhile, the Z-scheme type of heterojunctions can increase the carrier separation efficiency and maintain the high reduction ability of photogenerated electrons. As expected, the photocatalytic hydrogen evolution rate of the as-optimized ZnS/SnO2 sample can reach 2.17 mmol g?1 h?1, which is 15.5 times higher than that of the commercial ZnS. This work can offer a novel strategy for designing Z-scheme heterojunction as well as controlling the contact interface for boosted photocatalytic activity.  相似文献   

13.
In the photoelectrochemistry reaction, the electrode is most important. As a common electrode material, the metal oxide has a large band gap and high internal resistance, which is disadvantageous for photocatalytic hydrogen production. Metal selenide generally has a narrow band gap and low internal resistance, which is a promising new type of photocatalyst. A FeSe2/ZnSe heterojunction photocatalyst is constructed by loading ZnSe nanoparticles on FeSe2 nanorods. In this heterostructure, ZnSe is uniformly supported on the surface of FeSe2 to form a 0D/1D structure. Experiments have confirmed that the photoelectrochemical activity and photocatalytic H2 production rate of this heterojunction photocatalyst is greatly improved, and its optimum performance is three times of ZnSe in photoelectrochemical activity and 2.3 times in photocatalytic H2 production rate. Further analysis reveals that the internal resistance of the composite photocatalyst is greatly reduced due to the compositing of FeSe2, and the carrier separation efficiency is also improved. In this FeSe2/ZnSe heterojunction, the conduction band of ZnSe is more negative than that of FeSe2, and the photogenerated electrons generated on the conduction band of ZnSe can be transferred to that of FeSe2, thereby prolonging the carrier lifetime and improving photoelectrochemical activity. This work confirms that FeSe2/ZnSe is a very effective heterostructure, which avoids the addition of precious metals and rare earth metals and shows great application prospects.  相似文献   

14.
A designed type-II heterojunction photocatalyst, NiSe2/Cd0.5Zn0.5S (NiSe2/CZS), was successfully synthesized and it exhibits outstanding photocatalytic hydrogen evolution performance. The optimal loading amount of NiSe2 on Cd0.5Zn0.5S is 13 wt %, and the corresponding hydrogen production rate is approximately 121.01 mmol g?1 h?1 under visible light. The heterojunction structure between Cd0.5Zn0.5S and NiSe2 promoted the separation of photogenerated electron-hole pairs, effectively suppressed the photogenerated carrier recombination and endowed the material with excellent interfacial charge transfer properties, thus improving the photocatalytic performance.  相似文献   

15.
The coupling of two-dimensional (2D) layered materials is an effective way to realize photocatalytic hydrogen production. Herein, using first-principles calculations, the photocatalytic properties of GaN/CNs heterojunctions formed by two different graphite-like carbon nitride materials and GaN monolayer are discussed in detail. The results show that the GaN/C2N heterojunction can promote the effective separation of photogenerated electron and hole pairs, which is attributed to its type-II band orientation and high carrier mobility. However, the low overpotential of GaN/C2N for photocatalytic hydrogen production limits the photocatalytic performance. On this basis, we adjust the CBM position of the GaN/C2N heterojunction by applying an electric field to enhance its hydrogen evolution capability. In addition, the GaN/g-C3N4 is a type-I heterojunction, which is suitable for the field of optoelectronic devices. This work broadens the field of vision for the preparation of highly efficient photocatalysts.  相似文献   

16.
Visible-light photocatalytic water splitting for hydrogen evolution has attracted tremendous attention in past decades, but it still suffers from low solar-hydrogen conversion efficiency. In this paper, two-dimensional (2D) CdS was synthesized by the hydrothermal method, and 2D CoP nanosheets were synthesized by successive hydrothermal, oxidation and phosphodation process. Then 2D-2D CdS–CoP photocatalysts were formed by ultrasonically dispersing the mixed solution of CdS and CoP, and their heterostructure was confirmed by transmission electron microscopy, X-ray photoelectron spectroscopy, fluorescence spectrometer and so on. CdS–CoP with 2% CoP loading amounts exhibits a maximum photocatalytic performance of 56.3 mmolg−1h−1 under visible light irradiation, which is 11.3 times as high as bare CdS. The enhanced photocatalytic performance of CdS–CoP should be due to the following two points: (1) high catalytic activity of CoP; (2) highly efficient separation and transfer of electron-hole pairs photogenerated in CdS due to the synthesized 2D-2D heterostructure.  相似文献   

17.
The construction of semiconductor heterojunction for photocatalytic H2 production from water splitting is an efficient and environment-friendly technology. In this work, ZnO/BiOCl (ZBC) and Sn-doped ZnO/BiOCl (ZBC-S) photocatalysts with Z-scheme heterojunction were successfully prepared by simple hydrothermal method. The photocatalytic H2 evolution from water splitting by the as-prepared photocatalysts was investigated. The formation of ZnO/BiOCl heterojunction reduces the recombination probability of the photogenerated carriers. The impurity levels originated from Sn doping reduce the band gap width of ZnO and BiOCl to some extent, thereby enhancing the light absorption ability. The ZBC-S composite exhibits the best photocatalytic activity. In addition, the photocatalytic efficiency of H2 production was improved by sensitization with Eosin Y (EY) dye. The H2 production rate under simulated sunlight reaches 4146.77 μmol g?1 h?1, which is 27 times higher than that of pure ZnO. Finally, the Z-scheme electron transfer route in ZnO/BiOCl heterojunction was determined, and the photocatalytic H2 production mechanism of EY sensitized ZBC-S was proposed.  相似文献   

18.
The effective separation of photogenerated charge carriers, their transport and interfacial contact is of great significance for excellent performance of semiconductor based photocatalysts. Herein, we report the fabrication of two dimensional (2D) nanosheets heterojunction comprising of N-doped ZnO nanosheets loaded over graphitic carbon nitride (g-C3N4) nanosheets for enhanced photocatalytic hydrogen evolution. The prepared 2D-2D heterojunctions with varying amount of g-C3N4 nanosheets have been characterized by x-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and x-ray photoelectron spectroscopy (XPS) techniques. The optimized heterojunction photocatalyst with 30 wt% of g-C3N4 nanosheets (NZCN30) exhibit hydrogen evolution rate of 18836 μmol h?1 gcat?1 in presence of Na2S and Na2SO3 as sacrificial agents under simulated solar light irradiation. The enhanced photocatalytic performance of NZCN30 heterojunction has been supported well by photoluminescence and photoelectrochemical investigations, which shows the minimum recombination rate and high photoinduced current density, respectively. In addition, the existence of 2D-2D interfacial contact plays a major role in enhanced H2 evolution by high face-to-face contact surface area for separation of photogenerated charge carriers in space which facilitate their transfer for H2 generation. This work paves way for the development of 2D-2D heterojunctions for diverse applications.  相似文献   

19.
Ag-doped Bi2WO6-graphene based photocatalysts were found to exhibit hydrogen production activity. The performance of Bi2WO6-graphene based photocatalysts were investigated and optimized in this study. The activity can be further improved by Ag-doping. The morphology, surface chemistry, and phase structure of the photocatalysts were investigated by Field emission scanning electron microscopy, Transmission electron microscopy, X-ray photoelectron spectroscopy, Raman spectra, and X-ray diffraction. UV–vis diffuse reflectance spectroscopy and zeta potential were measured to study the optical properties, bandgap and dispersion stability of the photocatalysts. The effects of forming Bi2WO6-graphene contact and Ag doping on the light absorption, band gap, dispersion stability, and photocatalytic H2 production performance of the composite photocatalysts were evaluated. The improved photocatalytic performance is mainly owing to the Ag doping and high electrical conductivity of graphene.  相似文献   

20.
The present study reports about exploration of a multi-component photocatalytic system comprising of WO3, TiO2 and Fe2O3 with tandem n-n heterojunctions. The ternary WO3/TiO2/Fe2O3 nanocomposite with WO3 nanoparticles over the interfaces of Fe2O3 and TiO2 is synthesized by wet precipitation followed by thermal decomposition. The WO3/TiO2/Fe2O3 nanocomposite has an enhanced photocatalytic performance towards hydrogen generation by water splitting reaction under visible light irradiation, when compared to the Fe2O3/TiO2 system. A band gap of 2.10 eV, favouring visible light absorption was achieved with the distribution of WO3 nanopartcles over the interfaces of Fe2O3 and TiO2. The as prepared WTF heterojunction exhibited a maximum hydrogen production rate of 10.2 mL h−1 for a catalyst loading of 0.025 g mL−1. The enhanced photocatalytic performance is tested in presence of various sacrificial agents and proton source. In both cases, the higher photocatalytic efficiency is attributed to the more visible light harnessing ability and pronounced charge separation owing to the tandem n-n heterojunctions generated between TiO2 with WO3 and TiO2 with Fe2O3 semiconductors and enhancing the lifetime of the photogenerated electron-hole pairs.  相似文献   

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