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1.
Combining the strong localized surface plasmon resonance (LSPR) of metallic Ag and the chemically reactive Pt co-catalyst, the Ag–Pt bimetallic composite was prepared and then coated on the surface of the exfoliated defective graphitic carbon nitride nanosheets (C3Nx NS) for plasmon hot electron-mediated photocatalytic H2 evolution. Under the visible light irradiation, the sample of (1:2) Ag–Pt/C3Nx NS exhibits the highest activity (1.25 mmol g−1 h−1), which is 35.7 and 1.7 times higher than that of Ag/C3Nx NS and Pt/C3Nx NS, respectively. Moreover, the apparent quantum efficiency (AQE) of (1:2) Ag–Pt/C3Nx NS reaches 3.3% at 420 nm. The boosted photocatalytic capacity may be ascribed to the utilization of the advantages of the LSPR effect of Ag particles and the Schottky barrier between Pt and C3Nx NS, resulting in more electrons participate in the reduction reaction to boost the photocatalytic H2 evolution performance.  相似文献   

2.
Nanoporous TiO2 loaded with Pt and Ag was prepared by the dealloyed AlTiAgPt ribbons. The hydrogen generation rate via water splitting was measured for the photocatalytic performance. X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL), UV–vis diffuse reflectance spectroscopy (UV–vis) and Raman spectroscopy were employed to analyze the synergy among TiO2, Pt and Ag. The results indicate that the synthetic TiO2 shows an anatase structure and that the size of the Pt-rich phase, Ag and Ag-rich phase particles are approximately 6–8 nm. An abundance of pores with about 5 nm in size are distributed on the surface of TiO2, and obtained samples exhibit a larger specific surface area. The hydrogen evolution rate was approximately 1.85 mmol/h/g under full-spectrum irradiation for the dealloyed Al92Ti7.86Pt0.04Ag0.1 ribbons, which was greatly improved compared with that of the dealloyed Al92Ti7.9Ag0.1 ribbons. The analyses indicate that Ag could promote the visible light absorption and that Pt serves as an electron sink for the effective electron-hole pairs separation. Moreover, the appropriate Schottky barrier, formed among the Pt-rich phase, Ag-rich phase and TiO2, effectively suppresses the recombination of electron-hole pairs and improves the utilization of photo-generated electrons.  相似文献   

3.
In addition to the extended light absorption, the effective spatial charge separation is a crucial factor for highly efficient metal-oxide semiconductor-based photocatalysts. Herein, a rational design of metal-semiconductor-metal nano heterostructure for enhancing photocatalytic performance is proposed. The semiconductor nanoparticles are integrated with two metals in one single nano heterostructure. The disordered layers are induced on the surface of TiO2 to promote the light absorption capacity. More importantly, the n-n+ junction is fabricated at the contact region between crystalline TiO2 (n-TiO2) and disordered layers (n+-TiO2). Besides, the Schottky diode and Ohmic contact are formed on n-TiO2 and n+-TiO2, respectively. As a result, the existence of multi-junctions leads to the formation of multiple continuous built-in electric fields, thus remarkably accelerating the spatial separation of charge carriers. The resulting nano heterostructure with multi-junctions (Pt–TiO2–H–Ag) exhibits remarkably promoted photocatalytic performance. The maximum hydrogen generation rate of Pt–TiO2–H–Ag under solar illumination (18001.0 μmol/h/g) is 8.3, 9.3, and 1.5 times superior to that of Pt-loaded P25 (Pt–P25), Pt loaded TiO2 (Pt–TiO2), and hydrogenated Pt–TiO2 (Pt–TiO2–H), respectively. Moreover, the photocatalytic performance under visible illumination is significantly enhanced by Pt–TiO2–H–Ag. Specifically, the H2 generation rate of Pt–TiO2–H–Ag (2382.7 μmol/h/g) is about 15.1, 17.2, and 1.4 times higher than that of Pt–P25, Pt–TiO2, and Pt–TiO2–H, respectively. The corresponding apparent quantum efficiency of Pt–TiO2–H–Ag is 15.8% (420 nm). The nano heterostructure with multi-junctions also exhibits excellent stability after five cycles, remaining hydrogen evolution rates of 15581.5 and 2211.4 μmol/h/g under solar and visible illumination, respectively. This effective and controllable manufacturing strategy could provide new opportunities to simultaneously extend optical absorption and facilitate the spatial charge separation and transport of wide-bandgap metal-oxide semiconductors.  相似文献   

4.
Photocatalytic oxidation of toxic pollutants is a proficient technique to solve the problems associated with the treatment of bisphenol-A which is classified as 1B reprotoxic substance. In this paper, Ag2C2O4/Ag@GNS nanocomposite whereas Ag and graphene nanosheets (GNS) used as the charge carriers, which is combined through peroxymonosulfate (PMS) for the removal of bisphenol-A (BiP-A) for the first time. The XRD, UV-DRS, SEM, and TEM studies were performed to confirm the phase structure and the purity. Ag2C2O4/Ag@GNS nanocomposite exhibited superior photocatalytic performance and removal rate when compared with pure Ag2C2O4 and pure GNS. In Ag2C2O4/Ag@GNS photocatalyst, the deposited Ag on the surface of Ag2C2O4 rods effectively formed a metal and semiconductor heterostructure, thus photogenerated charge carriers were separated easily by the surface plasmon resonance effect (SPR) effect of noble Ag. Hence charge carriers lifetime has been extended to a great extent for the better photocatalytic performance. The experimental results confirmed that the ? O2?, ? OH, ? SO4? radicals were played major role in the photolysis process. Furthermore, the effect of the photocatalyst & PMS concentration, pH and co-existing ions towards the BiP-A degradation were studied in detail. According to the mass spectroscopy studies BiP-A pollutant was effectively deteriorated into smaller molecules and CO2, H2O. Furthermore, we have proposed the possible degradation pathway and photocatalytic mechanism for better understanding.  相似文献   

5.
This paper synthesized a novel Ag3PO4/P-g-C3N4 via a two-step chemical route i.e. microwave-assisted heating and ion-exchange procedures. The as-synthesized hybrid presented high efficiency for photocatalytic hydrogen production. Systematic investigation indicated that phosphorus was successfully doped into the g-C3N4 framework through microwave heating the mixture of melamine and NH4H2PO4 for 40 min, which increases the BET surface area, broadens the visible light response region, and elevates the separation efficiency of electron-hole pairs. The Ag3PO4 nanoparticles were decorated on the optimal P-g-C3N4 sample via an ion-exchange process. Due to the instability of Ag3PO4, the formed composite is actually Ag/Ag3PO4/P-g-C3N4 photocatalyst. The introduced Ag3PO4 nanoparticles further improves the charge separation efficiency of P-g-C3N4, but slightly affects the surface area and optical property, which highlights the key role of the separation efficiency of electron-hole pairs in photocatalytic reaction. The best Ag3PO4/P-g-C3N4 hybrid shows a photocatalytic H2 production rate of 1221 and 90.2 μmol g−1 h−1 under simulated sunlight and visible light, respectively. This value is 2.1 and 1.4 times greater than that of g-C3N4 and P-g-C3N4, respectively. Meanwhile, the Ag3PO4/P-g-C3N4 displayed high photocatalytic stability. A probable photocatalytic mechanism of the hybrid was also suggested.  相似文献   

6.
H2 dissociation barriers on Ag (111), Ag monolayer on WC (0001) (AgML/WC), Ag monolayer doped by Pt atom on WC (0001) (AgMLPt-d/WC) surface are decreasing from 1.07 to 0.03 eV. The ab initio atomistic thermodynamic data shows that at typical planar SOFC operating temperatures of 923–1073 K, under 100000-ppm pH2S/pH2, AgMLPt-d/WC can be sulfur free clean surface. Therefore, compared with traditional Nickel/Yttria-stabilized zirconia (Ni/YSZ) Solid Oxide Fuel Cells (SOFCs) anode, AgMLPt-d/WC shows high activity towards H2 dissociation and high tolerance of sulfur poisoning.  相似文献   

7.
In this work, bimetallic PtX (X = Sn, Cu) decorated graphene nanohybrids (PtX/G) were developed, which showed enhanced photocatalytic hydrogen evolution performance than that of Pt/G in Eosin Y sensitized H2 production system. The presence of Sn or Cu in PtX/G nanohybrids can remarkably improve the photogenerated charge separation efficiency and contribute to promoting the reduction of protons to molecular hydrogen in comparison to with noble metal Pt. Meanwhile, graphene acted as a more suitable electronic support to accelerate the migration of electrons from sensitizer to catalysts, owing to its higher electron mobility and larger surface area than other supports (such as carbon sphere, Al2O3 and SiO2). The optimal H2 evolution rate PtSn/G and PtCu/G was about 2.2 and 2.0 times higher than that of Pt/G. The apparent quantum efficiency (AQE) of PtSn/G and PtCu/G reached up to 12.46% and 11.06% under visible light irradiation (λ ≥ 420 nm), respectively.  相似文献   

8.
The synthesis of Ag3PO4/Ag was performed through in-situ deposition and photo-reduction processes with magnetic NiFe2O4 nanofibers towards enhanced photocatalysis performance and stability. NiFe2O4 inhibit the photoreduction of Ag3PO4 into Ag and resulted in high stability. The photocatalytic activity of Ag3PO4/Ag/NiFe2O4 samples was studied by methylene blue degrading under visible light irradiation. The Ag3PO4/Ag/NiFe2O4 photocatalyst with NiFe2O4 loading of 3% revealed good photocatalytic performance, high stability and quick degradation after 5 cycles. Photoluminescence spectra and photocurrent tests demonstrated that the formation of hetero-junction facilitated the separation of photo-generated carriers. The trapping experiments confirmed that h+ and ?OH were active species during the degradation process.  相似文献   

9.
Mesoporous-assembled SrTiO3 photocatalysts with different loaded metal co-catalysts (Au,Pt, Ag, Ni, Ce, and Fe) synthesized by the single-step sol–gel method with the aid of a structure-directing surfactant were tested for the photocatalytic activity of hydrogen production from a methanol aqueous solution under both UV and visible light irradiation. The Au, Pt, Ag, and Ni loadings had a positive effect on the photocatalytic activity enhancement, whereas the Ce and Fe loadings did not. The best loaded metal was found to be Au due to its electrochemical properties compatible with the SrTiO3-based photocatalyst and its visible light harvesting enhancement. A 1 wt.% Au-loaded SrTiO3 photocatalyst exhibited the highest photocatalytic hydrogen production activity with a hydrogen production rate of 337 and 200 μmol h−1 gcat−1 under UV and visible light irradiation, respectively. The hydrogen diffusivity from the liquid phase to the gas phase also significantly affected the photocatalytic hydrogen production efficiency. An increase in the hydrogen diffusability led to an increase in the photocatalytic hydrogen production efficiency.  相似文献   

10.
In this study, a ternary photocatalyst named Ag–AgBr/g-C3N4/ZIF-8 (A/g/Z) was prepared by ionic liquid assisted in-situ growth method. The structure and composition of samples are studied by means of XRD, SEM, XPS, TEM, EIS, etc. The AgBr prepared by ionic liquid assisted method has good dispersion, and the protonated carbon nitride has better specific surface area and morphology structure. The structure of the composites is optimized by modifying g-C3N4 with MOFs and noble metals, and the existence of Ag+ can play a bridging role, so as to form multi-path electronic transmission route. The high efficiency of electron transfer greatly improved the efficiency of hydrogen evolution. It is worth noting that the surface plasmon resonance (SPR) effect produced by silver ions on the surface of g-C3N4 can improve the absorption of visible light. The A (1.1)/g/Z (6.5) exhibit high hydrogen evolution efficiency (2058 μmol g?1 h?1, which is 49 times than g-C3N4) at the absence of Pt co-catalyst. Furthermore, the transient photocurrent density of the composites is much higher than that of g-C3N4 and AgBr, the semicircle radius of EIS is also less than both. Through the five cycle experiment, the photocatalytic efficiency of the composite material remained above 91%.  相似文献   

11.
Although black phosphorous (BP) and its derived materials have shown great potential for application in photocatalytic H2 evolution reaction (HER), their HER activity and stability still remains unsatisfied mainly due to the insufficient charge separation, the lack of surface active sites, and the defect-riched nature of BP. Herein, we report that BP nanosheets decorated with in situ grown Pt (BP NSs/Pt) could act as a highly efficient catalyst for photocatalytic H2 evolution in an Erythrosin B (ErB)-sensitized system under visible light irradiation (≥450 nm) in the presence of triethanolamine (TEOA) as sacrificial electron donor. It is found that BP NSs can provide large surface area for the confined growth of Pt nanoparticles with a high dispersion and a reduced size but also stabilize the loaded Pt nanoparticles by covalent bonds at the BP NSs/Pt interfaces. Moreover, BP NSs offer a fast electron transfer pathway to facilitate the photocatalytic HER over in situ grown Pt catalyst. As a result, BP NSs/Pt catalyst exhibits ∼6 times higher H2 evolution activity than free Pt nanoparticles and an apparent quantum yield (AQY) of 0.57% at 500 nm irradiation in ErB-TEOA system. This work indicates the potential of BP NSs as an effective 2D matrix to construct numerous high performance photocatalysts and photocatalytic systems.  相似文献   

12.
The options of transition metals as co-catalysts for photocatalytic H2S splitting are restricted to some noble metals and related compounds which have noticeable achievements despite their high prices. Substituting with cheap transition metals and downsizing the size to single atom level are economic ways to lower the cost. Herein, the s-triazine graphite-like carbon nitride sheet g-C3N4 (001) is chosen as the model to study the performances of 3d and 4d transition metal single atoms (TMSA = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd) in H2S splitting based on density functional theory (DFT) calculations. It is found that low-cost transition metals with industrial relevance (Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Tc, Cd) are completely comparable with noble metals (Ru, Rh, Pd, Ag). Among them, V and Nb are the most promising co-catalysts with good thermodynamic stabilities, favorable responses to visible light, high photoinduced electron-hole separation efficiencies, sufficient potentials for H2S splitting, and low energy barriers for H2S dissociation into H2 and S. The noticeable improved activities of V/g-C3N4 and Nb/g-C3N4 are attributed to the formation of strong interfacial chemical bonds which could promote electrons transferring to H2S derivates. In addition, the introduction of photoinduced electrons could further improve the activities of V/g-C3N4 and Nb/g-C3N4 with more electrons transferring to H2S derivates. It is expected that this work could provide a helpful guidance to choose appropriate TMSA co-catalysts as references for H2S splitting.  相似文献   

13.
Bimetal PtAu modifying nanoporous TiO2 composites are prepared by dealloying. X-ray diffraction is used to determine the phase constitution. The specific surface area and mesoporous pores are measured by Brunauer-Emmett-Teller. X-ray photoelectron spectroscopy, photoluminescence spectroscopy, UV–Vis diffuse reflectance spectroscopy and Raman spectroscopy are employed to analyse the mutual synergy between Pt and Au. The hydrogen generation rate is measured to determine the photocatalytic performance. The results reveal that TiO2 is the anatase structure and possess a sea cucumber-like morphology with a large specific surface area. The hydrogen generation rate is 1.745 mmol h?1 g?1 for the dealloyed Al92Ti7.86Pt0.04Au0.1 ribbons under the full spectrum irradiation. This value is 29.6 times, 4.4 times and 1.8 times those of the dealloyed Al92Ti8, Al92Ti7.9Au0.1, and Al92Ti7.96Pt0.04 ribbons, respectively. The above results indicate that the addition of a small amount of Au and Pt significantly enhances the photocatalytic activity for H2 production. The Au promotes the absorption of visible light, and Pt serve as an electron sink for effective electron-hole pairs separation during the photocatalytic process. It is a feasible and an effective strategy to take full advantages of respective virtues of noble metals and their strong interactions to enhance photocatalytic activity.  相似文献   

14.
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   

15.
We demonstrate a general method for the synthesis of biomass-derived hierarchical porous CdS/M/TiO2 (M = Au, Ag, Pt, Pd) ternary heterojunctions for efficient photocatalytic hydrogen evolution. A typical biomass—wood are used as the raw sources while five species of wood (Fir, Ash, White Pine, Lauan and Shiraki) are chosen as templates for the synthesis of hierarchical porous TiO2. The as-obtained products inherited the hierarchical porous features with pores ranging from micrometers to nanometers, with improved photocatalytic hydrogen evolution activity than non-templated counterparts. Noble metals M (M = Pt, Au, Ag, Pd) and CdS are loaded via a two-step photodeposition method to form core (metal)/shell (CdS) structures. The photocatalytic modules—CdS(shell)/metal (core)/TiO2 heterostructures, have demonstrated to increase visible light harvesting significantly and to increase the photocatalytic hydrogen evolution activity. The H2 evolution rates of CdS/Pd/TiO2 ternary heterostructures are about 6.7 times of CdS/TiO2 binary heterojunctions and 4 times higher than Pd/CdS/TiO2 due to the vertical electron transfer process. The design of such system is beneficial for enhanced activity from morphology control and composition adjustment, which would provide some new pathways for the design of promising photocatalytic systems for enhanced performance.  相似文献   

16.
The development of high-efficiency and low-cost photocatalysts in photocatalytic H2 evolution systems from water remains challenging. The substitution of a noble metal as the co-catalyst is still one of the important and meaningful issues in this field. Herein, we report a series of CaIn2S4 catalysts combined with Ni2P, which acts as the co-catalyst, for boosting photocatalytic hydrogen evolution under visible light. The integrated system of the Ni2P/CaIn2S4 composite exhibited high efficiency and durability, which were even higher than those of Pt decorated catalysts. The promoting effect of Ni2P can be ascribed to its excellent reductive ability and analogous metallic character, which can accelerate the transfer and consumption of the photo-generated electrons. Moreover, based on the surface photo-voltage technique and electrochemical tests, the unique mechanism of Ni2P for the movement of photo-generated charges during the photocatalysis process is proposed for the first time.  相似文献   

17.
The two-step decoration of the Ag nanoparticles supported on carbon black (Ag/C) with Au and Pt, the electrooxidation of glycerol on the Pt/Au/Ag/C catalysts in alkaline solution, and the effect of the amounts of Au and Pt on the catalytic activity of Pt/Au/Ag/C are investigated. The decoration of Ag/C is performed by electrochemically depositing a small amount of Au and then Pt on Ag/C, and the Ptx/Auy/Ag100/C catalysts with different x:y:100 ratios (0.15 ≤ x ≤ 1.9 and 0.2 ≤ y ≤ 1.5) are obtained. Physical and electrochemical characterizations reveal that small parts of the Ag surfaces are covered by the deposited Au and Pt. Ptx/Auy/Ag100/C mainly shows Pt-relevant behaviors in glycerol oxidation, and Pt1.3/Auy/Ag100/C exhibits high catalytic activities. The results reveal that the surface decoration is a useful method of fabricating efficient ternary catalysts at low cost.  相似文献   

18.
A plasmonic photocatalyst is designed and synthesized by coating TiO2 nanoparticles onto the surface of Ag nanorods (Ag NRs), namely one-dimensional TiO2@Ag NRs photocatalyst. Materials characterizations suggest that the as-prepared catalysts consist of a uniform and high crystalline anatase nanocrystals and highly conductive Ag nanorod. It delivers remarkable visible-light photocatalytic performance in simultaneous H2 evolution and decomposition of methyl orange (MO) due to the synergetic effects of plasmonic resonance under visible light irradiation, a matched heterojunction, high surface area and large conductivity.  相似文献   

19.
Nanostructured conducting polymeric materials are beneficial for electron conduction and mass transport, showing high photocatalytic performance under visible light. Herein, we report a colloidal synthesis of copper and copper oxides (Cu2O) modified polypyrrole nanofibers (PPy) heterostructures, which demonstrates significantly high photocatalytic H2 generation under visible light. The presence of Cu nanoparticles (NPs) of 50 nm and cubic shaped Cu2O nanoparticles of size 200 nm endows the heterostructures with a large specific surface area as well as good dispersion of nanoparticles on PPy nanofibers allows the migration of electron during catalysis. Cu2O/PPy exhibits excellent H2 production (67 mmol h−1) which is 12 times higher than pure PPy (5.7 mmol h−1). The high catalytic activity of Cu2O/PPy heterostructure provides a fervent alternative to noble metal-based catalysts for the hydrogen generation and water splitting.  相似文献   

20.
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   

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