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1.
《Ceramics International》2017,43(10):7901-7907
g-C3N4 as a new metal-free photocatalytic material for water splitting has attracted much attention in recent years, but its photocatalytic efficiency needs further improvement. Here we synthesized novel C60/graphene/g-C3N4 composite photocatalytic materials with high hydrogen generation ability for water splitting under visible light radiation (λ>420 nm). These materials take full advantage of the electron conduction expressing of graphene and the superior-strong electron-attracting ability of C60. The mutually-reinforcing synergy between graphene and C60 improves the migration and utilization efficiency of photo-generated electrons and accelerates the separation of photo-generated charges, thus significantly enhancing the hydrogen generation capacity of g-C3N4. The hydrogen production amount and rate of C60/graphene/g-C3N4 (10 mg/L C60 and graphene) after 10 h are 5449.5 µmol/g and 545 µmol/g/h, which is 539.6 times of pure g-C3N4 under the same condition. The values are 50.8 and 4.24 times of graphene/g-C3N4 (10 mg/L graphene) and C60/g-C3N4 (10 mg/L C60), respectively. The apparent quantum yield of C60/graphene/g-C3N4 (10 mg/L C60 and graphene) in 97 h is about 7.2%. The improvement of hydrogen generation activity in 97 h suggests the high long-time stability of C60/graphene/g-C3N4 in photocatalytic water spitting. The photocatalytic ability of C60/graphene/g-C3N4 can be controlled by regulating the addition of graphene and C60. The mutually-reinforcing synergy between graphene and C60 was proved by X-ray photoelectron spectroscopy, photoluminescence spectrum and organic electron acceptors of MV2+. Thus, the joint action of C60 and graphene promotes the migration, separation and utilization of photo-generated electrons, which is responsible for the significant enhancement of photocatalytic performance.  相似文献   

2.
《Ceramics International》2016,42(16):18443-18452
Highly efficient visible-light-driven heterojunction photocatalysts, spindle-shaped nanoporous TiO2 coupled with graphitic g-C3N4 nanosheets have been synthesized by a facile one-step solvothermal method. The as-prepared photocatalysts were characterized by X-ray diffraction (XRD), energy dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N2 adsorption-desorption analysis and UV–vis diffuse reflectance spectrometry (DRS), proving a successful modification of TiO2 with g-C3N4. The results showed spindle-shaped nanoporous TiO2 microspheres with a uniform diameter of about 200 nm dispersed uniformly on the surface of graphitic g-C3N4 nanosheets. The g-C3N4/TiO2 hybrid materials exhibited higher photocatalytic activity than either pure g-C3N4 or nanoporous TiO2 towards degradation of typical rhodamine B (RhB), methyl blue (MB) and methyl orange (MO) dyes under visible light (>420 nm), which can be largely ascribed to the increased light absorption, larger BET surface area and higher efficient separation of photogenerated electron–hole pairs due to the formation of heterostructure. In addition, the possible transferred and separated behavior of electron–hole pairs and photocatalytic mechanisms on basis of the experimental results are also proposed in detail.  相似文献   

3.
《Ceramics International》2017,43(16):13581-13591
The nanocomposites of WO3 nanoparticles and exfoliated graphitized C3N4 (g-C3N4) particles were prepared and their properties were studied. For this purpose, common methods used for characterization of solid samples were completed with dynamic light scattering (DLS) method and photocatalysis, which are suitable for study of aqueous dispersions.The WO3 nanoparticles of monoclinic structures were prepared by a hydrothermal method from sodium tungstate and g-C3N4 particles were prepared by calcination of melamine forming bulk g-C3N4, which was further thermally exfoliated. Its specific surface area (SSA) was 115 m2 g−1.The nanocomposites were prepared by mixing of WO3 nanoparticles and g-C3N4 structures in aqueous dispersions acidified by hydrochloric acid at pH = 2 followed by their separation and calcination at 450 °C. The real content of WO3 was determined at 19 wt%, 52 wt% and 63 wt%. It was found by the DLS analysis that the g-C3N4 particles were covered by the WO3 nanoparticles or their agglomerates creating the nanocomposites that were stable in aqueous dispersions even under intensive ultrasonic field. Using transmission electron microscopy (TEM) the average size of the pure WO3 nanoparticles and those in the nanocomposites was 73 nm and 72 nm, respectively.The formation of heterojunction between both components was investigated by UV–Vis diffuse reflectance (DRS) and photoluminescence (PL) spectroscopy, high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), photocatalysis and photocurrent measurements. The photocatalytic decomposition of phenol under the LED source of 416 nm identified the formation of Z-scheme heterojunction, which was confirmed by the photocurrents measurements. The photocatalytic activity of the nanocomposites decreased with the increasing content of WO3, which was explained by shielding of the g-C3N4 surface by bigger WO3 agglomerates. This study also demonstrates a unique combination of various characterization techniques working in solid and liquid phase.  相似文献   

4.
A series of g-C3N4–Sb2S3/Sb4O5Cl2 (SCL-CX) composite photocatalysts were successfully prepared via a hydrothermal method. The as-prepared materials were characterized by TM3000, powder X-ray diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS) and UV–vis diffuse reflectance spectra (UV–vis DRS). The obtained photocatalyst showed higher photocatalytic activity than pure g-C3N4, Sb4O5Cl2 and Sb2S3/Sb4O5Cl2 (SCL). The optimum photocatalytic of the composite with the mass of 170 mg g-C3N4 and a degradation efficiency up to 95% for methyl orange (MO) under visible light was achieved within 60 min. The enhanced photocatalytic performance could be attributed to the stronger absorption in the visible region and the more efficient electron–hole separation.  相似文献   

5.
BiPO4/g-C3N4 with different amounts of BiPO4 was prepared through wet impregnation with calcination method. The BiPO4/g-C3N4 showed large surface area (172.9 m2 g 1) and the incorporation of BiPO4 caused a red-shift of g-C3N4 in visible light. The photocatalytic degradation of toluene over the samples was investigated. The degradation of toluene could get 82% in BiPO4/g-C3N4 photocatalysts under optimum reaction conditions. The BiPO4/g-C3N4 exhibited a higher photocatalytic activity than pure g-C3N4 or BiPO4. The improved photoactivity of BiPO4/g-C3N4 could be attributed to strong absorption in visible light and effective separation of photo-induced hole-electron pairs between BiPO4 and g-C3N4.  相似文献   

6.
《Ceramics International》2016,42(3):4063-4071
The graphitic carbon nitride (g-C3N4) was rapidly synthesized via direct high-energy microwave heating approach. During the preparation process, only low-cost melamine and artificial graphite powders were used, without any metal catalysts or inert protective gas. The microstructure was investigated by using X-ray diffraction (XRD), Flourier transformed infrared (FT-IR), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM). The spectra of XRD and HRTEM indicated that the obtained g-C3N4 had a high crystallinity. The optical spectra covering Photoluminescence (PL) and Ultraviolet-visible (UV–vis) were also measured at room temperature. PL peak and UV–vis absorption edge of the g-C3N4 were shown at 455 nm and 469 nm, respectively, indicating visible-light photocatalytic property. Finally, the photocatalytic activity of g-C3N4 was investigated and evaluated as photocatalyst for the photo-degradation of Rhodamine B (RhB) and Methyl Orange (MO) in aqueous solution under visible-light (λ>420 nm) irradiation, respectively. Results indicated that the g-C3N4 sample displayed an excellent performance of removing of RhB and MO due to the improved crystallinity and large surface area of 126 m2/g. After the visible-light photocatalytic reaction for 40 min, the decolorization ratios of RhB and MO reached up to 100% and 94.2%, respectively.  相似文献   

7.
A novel molybdenum disulfide (MoS2) and graphitic carbon nitride (g-C3N4) composite photocatalyst was synthesized using a low temperature hydrothermal method. MoS2 nanoparticles formed on g-C3N4 nanosheets greatly enhanced the photocatalytic activity of g-C3N4. The photocatalyst was tested for the degradation of methyl orange (MO) under simulated solar light. Composite 3.0 wt.% MoS2/g-C3N4 showed the highest photocatalytic activity for MO decomposition. MoS2 nanoparticles can increase the interfacial charge transfer and thus prevent the recombination of photo-generated electron–hole pairs. The novel MoS2/g-C3N4 composite is therefore shown as a promising catalyst for photocatalytic degradation of organic pollutants using solar energy.  相似文献   

8.
Molybdenum doped graphitic carbon nitride (g-C3N4) catalysts were prepared by a simple pyrolysis method using melamine and ammonium molybdate as precursors. The characterization results indicated that the obtained Mo-doped g-C3N4 catalysts had worm-like mesostructures with higher surface area. Introduction of Mo species can effectively extend the spectral response property and reduce the recombination rate of photogenerated electrons and holes. CO2 photocatalytic reduction tests showed that the Mo-doped g-C3N4 catalysts exhibited considerably higher activity (the highest CO and CH4 yields of 887 and 123 μmol g 1-cat., respectively, after 8 h of UV irradiation.) compared with pure g-C3N4 from melamine.  相似文献   

9.
《Ceramics International》2016,42(16):18521-18528
In this work, ultrathin graphene-like carbon nitride nanosheets with rich nanoporous and excellent hydrophilic characteristics were synthesized by a simple and effective thermal exfoliation of bulk g-C3N4. In order to fully understand the effect of thermal exfoliation conditions on the texture, surface state, and photocatalytic activity of the resulting g-C3N4, a series of exfoliated g-C3N4 were prepared by adjusting the thermal exfoliation temperature and time. The detailed characterization and analysis distinctly suggested that increasing exfoliation temperature led to a large number of nitrogen vacancies and increased specific surface area, further prolonging exfoliation time, the thermal exfoliation degree was enhanced, more carbon vacancies and enlarged pore volume formed in the resulting products. Further, the exfoliation degree and photocatalytic ability of the resultant products were enhanced by increasing thermal exfoliation temperature and time. The optimized ultrathin graphene-like carbon nitride nanosheets exhibited a 89.6% degradation efficiency for Rh6G only in 10 min, which was much faster than other such nanosheets reported in previous literature.  相似文献   

10.
Tin dioxide nanoparticles were prepared in the presence of graphitized carbon nitride (g-C3N4) forming nanocomposites with different contents of SnO2 up to 40 %. G-C3N4 was synthetized by heating of melamine at 550 °C in the open air and Sn2+ ions were precipitated by sodium hydroxide in g-C3N4 aqueous dispersions. Resulting mixtures were dried by freezing at ?20 °C and calcined at 450 °C to obtain SnO2/g-C3N4 nanocomposites.The nanocomposites were characterized by common characterization methods in solid state and in their aqueous dispersions using dynamic light scattering (DLS) analysis and photocatalysis. SnO2 nanoparticles in the nanocomposites were found to have an average size of 4 nm, however, those precipitated without g-C3N4 had an average size of 14 nm. Separation of photoinduced electron and holes via heterojunction between SnO2 and g-C3N4 was demonstrated by photocatalytic decomposition of Rhodamine B (RhB) under LED visible irradiation (416 nm) and photocurrent measurements. The most photocatalytically active nanocomposite contained 10 % of SnO2. Graphitized carbon nitride was assumed to serve as a template structure for the preparation of SnO2 nanoparticles with a narrow size distribution without using any stabilizing additives.  相似文献   

11.
《Ceramics International》2016,42(3):4158-4170
The development of a graphitic carbon nitride (g-C3N4) photocatalyst is of great importance to a variety of visible utilization application fields. The desired high efficiency can be achieved by employing well-controlled g-C3N4 nanostructures. In this study, we successfully synthesized high surface area g-C3N4 nanowires and nanofibers using a cyanuric chloride and melamine precursor dispersed in a solvothermal reaction and with a subsequent calcination step. The obtained novel nanowire product had a diameter of 10–20 nm and a length of several hundreds of nanometers, while the nanofibers revealed fibrous nanostructures of randomly dispersed fibers with an average diameter of ~15 nm. The adsorption and photocatalytic experimental results indicated that the as-prepared nanowires and nanofibers showed enhanced activities compared with bulk g-C3N4. Based on our experimental results, a possible photocatalytic mechanism with hydroxyl and superoxide radical species as the main active species in photocatalysis was proposed. Moreover, our strategy may provide progress toward the design and practical application of 1D g-C3N4 nanostructures in the adsorption and photocatalytic degradation of pollutants.  相似文献   

12.
《Ceramics International》2016,42(16):18116-18123
A series of onion-like carbon modified porous g-C3N4 (OLC/pg-C3N4) composites have been fabricated by a simple ultrasonic adsorption approach. The resultant OLC/pg-C3N4 composites exhibit excellent photocatalytic activity and stability towards the degradation of the dyes and phenol in aqueous solution under visible-light irradiation. The composite with 2.0 wt% OLC content shows the optimal photocatalytic activity for degrading rhodamine B (RhB), its rate constant is about three times that of pure pg-C3N4. The improved photocatalytic activity is mainly attributed to the synergetic effect of pg-C3N4 and OLC, including larger surface area, stronger visible light adsorption and efficient separation of photogenerated electrons and holes. Moreover, a possible mechanism of photocatalytic reaction over OLC/pg-C3N4 composite is proposed.  相似文献   

13.
A series of g-C3N4/ZnAl2O4 composites were prepared using a conventional calcination method and the heterostructures were systematically characterized. It was found that the combination of g-C3N4 with ZnAl2O4 significantly improve their photocatalytic activities. The optimum photocatalyst of composite is at 5% (wt%) of ZnAl2O4, whose degradation efficiency for methyl orange (MO) was 96% within 120 min under visible-light irradiation. The formation of heterojunction between g-C3N4 and ZnAl2O4 can facilitate efficient charge separation of photogenerated electron-hole pairs, which were confirmed by electrochemical impedance spectroscopy (EIS). As a result, the photocatalytic properties of composites were enhanced.  相似文献   

14.
Surface-enhanced Raman scattering (SERS) substrates with high SERS activity and stability are important for SERS sensors. A facile method was developed to fabricate efficient and stable SERS substrates by combining Ag nanoparticles (NPs) and micro-scale sheeted graphitic carbon nitride (g-C3N4). The g-C3N4/Ag NPs hybrid could provide a great number of hot spots and concentrated the analyte by the π–π stacking interaction between analyte molecules and g-C3N4, making a dramatic Raman enhancement. Moreover, the g-C3N4/Ag NPs hybrid uniformly immobilized Ag NPs on the surface and edges of g-C3N4 sheets by an interaction between Ag NPs and g-C3N4, leading to much improved long-term stability. This could be explained in terms of the electron–donor effect of g-C3N4, which was further confirmed by density functional theory calculations. The inherent Raman enhancing effect of g-C3N4 itself also contributed to the total SERS responses. Due to multiple enhancement contributions, the g-C3N4/Ag NPs hybrid exhibited a strong Raman enhancement effect for with an enhancement factor of 4.6 × 108 (evaluated by using crystal violet as a probe), and possessed wide adaptability from dyes, pesticides to bio-molecules.  相似文献   

15.
《Ceramics International》2016,42(8):9796-9803
The improved photocatalyst carbon-doped WO3/TiO2 mixed oxide was synthesized in this study using the sol–gel method. The catalyst was thoroughly characterized by X-ray diffraction (XRD), diffuse reflectance UV–vis spectroscopy, N2 adsorption desorption analysis, scanning electron microscopy coupled with energy dispersive X-ray analysis (SEM/EDX), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The photocatalytic efficiency of the prepared materials was evaluated with respect to the degradation of sodium diclofenac (DCF) in a batch reactor irradiated under simulated solar light. The progress of the degradation process of the drug was evaluated by high-performance liquid chromatography (HPLC), whereas mineralization was monitored by total organic carbon analysis (TOC) and ion chromatography (IC). The results of the photocatalytic evaluation indicated that the modified catalyst with tungsten and carbon (TWC) exhibited higher photocatalytic activity than TiO2 (T) and WO3/TiO2 (TW) in the degradation and mineralization of diclofenac (TWC>TW>T). Complete degradation of diclofenac occurred at 250 kJ m−2 of accumulated energy, whereas 82.4% mineralization at 400 kJ m−2 was achieved using the photocatalytic system WO3/TiO2-C. The improvement in the photocatalytic activity was attributed to the synergistic effect between carbon and WO3 incorporated into the TiO2 structure.  相似文献   

16.
Graphitic carbon nitride (g-C3N4) consists of two-dimensional sheets of carbon and nitrogen atoms. Films of g-C3N4 were prepared by evaporating guanidine carbonate at four different substrate temperatures. The optical absorption band of the films appears at 3.3 eV and the optical energy gaps are calculated to be 2.83–2.90 eV. Band intensity increases with increasing substrate temperature, but the energetic band position does not shift. The photocurrent of g-C3N4 films can be observed by irradiation with monochromatic light. While the photosensitivity spectra are in almost complete correspondence with the optical absorption spectra, it is also found that the photocurrent is generated by irradiation at photon energies below the optical energy gap down to 2.5 eV.  相似文献   

17.
《Ceramics International》2019,45(12):15178-15187
Graphitic carbon nitride (g-C3N4) has attracted increasing interest as a visible-light-active photocatalyst. In this study, saddle-curl-edge-like g-C3N4 nanosheets were prepared using a pellet presser (referred to as g-CN P nanosheets). Urea was used as the precursor for the preparation of g-C3N4. Thermal polymerization of urea in a pellet form significantly affected the properties of g-C3N4. Systematic investigations were performed, and the results for the modified g-C3N4 nanosheets are presented herein. These results were compared with those for pristine g-C3N4 to identify the factors that affected the fundamental properties. X-ray diffraction analysis and high-resolution transmission electron microscopy revealed a crystallinity improvement in the g-CN P nanosheets. Fourier-transform infrared spectroscopy provided clear information regarding the fundamental modes of g-C3N4, and X-ray photoelectron spectroscopy (XPS) peak-fitting investigations revealed the variations of C and N in detail. The light-harvesting property and separation efficiency of the photogenerated charge carriers were examined via optical absorption and photoluminescence studies. The valence band edge and conduction band edge potentials were calculated using XPS, and the results indicated a significant reduction in the bandgap for the g-CN P nanosheets. The Brunauer–Emmett–Teller surface area increased for the g-CN P nanosheets. The photocatalytic degradation performance of the g-CN P nanosheets was tested by applying a potential and using the classical dye Rhodamine B (RhB). The RhB dye solution was almost completely degraded within 28 min. The rate constant of the g-CN P nanosheets was increased by a factor of 3.8 compared with the pristine g-C3N4 nanosheets. The high crystallinity, enhanced light absorption, reduced bandgap, and increased surface area of the saddle-curl-edge-like morphology boosted the photocatalytic performance of the g-CN P nanosheets.  相似文献   

18.
In this contribution, the effect of hydrogenation conditions atmosphere (temperature and time) on physicochemical properties and photocatalytic efficiency of graphitic carbon nitride (g-C3N4, gCN) was studied in great details. The changes in the morphology, chemical structure, optical and electrochemical properties were carefully investigated. Interestingly, the as-modified samples exhibited boosted photocatalytic degradation of Rhodamine B (RhB) with the assistance of visible light irradiation. Among modified gCN, the sample annealed at 500 °C for 4 h (500-4) in H2 atmosphere exhibited the highest photocatalytic activity—1.76 times higher compared to pristine gCN. Additionally, this sample presented high stability and durability after four cycles. It was noticed that treating gCN with hydrogen at elevated temperatures caused the creation of nitrogen vacancies on gCN surfaces acting as highly active sites enhancing the specific surface area and improving the mobility of photogenerated charge carriers leading to accelerating the photocatalytic activity. Therefore, it is believed that detailed optimization of thermal treatment in a hydrogen atmosphere is a facile approach to boost the photoactivity of gCN.  相似文献   

19.
Graphitic carbon nitride(g-C3N4) sub-microspheres was first prepared via a facile microwave synthesis through polymerization reaction between cyanuric chloride(C3N3Cl3) and sodium azide (NaN3) using acetonitrile (ACN) as solvent, and the prepared samples were investigated by XRD, FTIR, XPS, SEM, TEM, UV–Vis, PL, TGA and BET, respectively. The results show that g-C3N4 are insoluble to conventional solvents except DMSO, and it exhibits a good chemical stability, thermal stability(< 650 °C), particle size with 0.076–0.137 μm in diameter, surface area of 89.1 m2/g and a band gap of 2.41 eV. Additionally, g-C3N4 prepared by microwave method also displays higher thermal stability, smaller particle radius, larger surface area, lower band gap and stronger emission intensity than traditional solvothermal method. Finally, the effect of microwave on the behavior of C3N4 sub-microsphere is proposed as well.  相似文献   

20.
《Ceramics International》2020,46(13):21431-21438
The solar light sensitive g-C3N4/TiO2 heterojunction photocatalysts containing 20, 50, 80, and 90 wt% graphitic carbon nitride (g-C3N4) were prepared by growing Titania (TiO2) nanoparticles on the surfaces of g-C3N4 particles via one step hydrothermal process. The hydrothermal reactions were allowed to take place at 110 °C at autogenous pressure for 1 h. Raman spectroscopy analyses confirmed that an interface developed between the surfaces of TiO2 and g-C3N4 nanoparticles. The photocatalyst containing 80 wt% g-C3N4 was subsequently heat treated 1 h at temperatures between 350 and 500 °C to improve the photocatalytic efficiency. Structural and optical properties of the prepared g-C3N4/TiO2 heterojunction nanocomposites were compared with those of the pristine TiO2 and pristine g-C3N4 powders. Photocatalytic activity of all the nanocomposites and the pristine TiO2 and g-C3N4 powders were assessed by the Methylene Blue (MB) degradation test under solar light illumination. g-C3N4/TiO2 heterojunction photocatalysts exhibited better photocatalytic activity for the degradation of MB than both pristine TiO2 and g-C3N4. The photocatalytic efficiency of the g-C3N4/TiO2 heterojunction photocatalyst heat treated at 400 °C for 1 h is 1.45 times better than that of the pristine TiO2 powder, 2.20 times better than that of the pristine g-C3N4 powder, and 1.24 times better than that of the commercially available TiO2 powder (Degussa P25). The improvement in photocatalytic efficiency was related to i) the generation of reactive oxidation species induced by photogenerated electrons, ii) the reduced recombination rate for electron-hole pairs, and iii) large specific surface area.  相似文献   

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