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1.
In this work, a series of Ag/AgX (X = Cl, Br, I)/g-C3N4 (Ag/AgX/CN) composites were successfully fabricated by an in-situ solid phase method. The morphology and structure, photoluminescence and photoelectrochemical properties of composites were investigated in detail. The as-prepared Ag/AgX/CN composites were used as H2 evolution photocatalysts under visible-light irradiation with a sacrificial agent. The experimental results revealed that Ag/AgI/CN-4 composite possesses highest-H2 evolution rate (up to 59.22 μmol g−1 h−1) which are approximately 31 times higher than that of pure g-C3N4 (1.94 μmol g−1 h−1). In addition, Ag/AgCl/CN-4 and Ag/AgBr/CN-4 composites also present high photocatalytic activities yielding, 26.39 and 18.05 μmolH2 g−1 h−1, respectively. The enhanced photocatalytic activities of Ag/AgI/CN-4 composite might be attributed to the synergistic effect between Ag/AgI nanoparticles and g-C3N4 and the localized surface plasmon resonance effect of metallic Ag. Moreover, Ag/AgI/CN-4 composite showed excellent recyclability and stability after five cycling photocatalytic tests (about 25 h). Furthermore, the possible photocatalytic mechanism of Ag/AgI/CN composites is proposed.  相似文献   

2.
In this report, a novel g-C3N4/Au/BiVO4 photocatalyst has been prepared successfully by assembling gold nanoparticles on the interface of super-thin porous g-C3N4 and BiVO4, which exhibits outstanding photocatalytic performance toward hydrogen evolution and durable stability in the absence of cocatalyst. FESEM micrograph analysis suggested that the intimate contact between Au, BiVO4, and g-C3N4 in the as-developed photocatalyst allows a smooth migration and separation of photogenerated charge carriers. In addition, the XRD, EDX and XPS analysis further confirmed the successful formation of the as-prepared g-C3N4/Au/BiVO4 photocatalyst. The photocatalytic hydrogen production activity of the developed photocatalyst was evaluated under visible-light irradiation (λ > 420 nm) using methanol as a sacrificial reagent. By optimizing the 5-CN/Au/BiVO4 composite shows the highest H2 evolution rate (2986 μmolg−1h−1), which is 15 times higher than that of g-C3N4 (199 μmolg−1h−1) and 10 time better than bare BiVO4 (297 μmolg−1h−1). The enhancement in photocatalytic activity is attributed to efficient separation of the photoexcited charges due to the anisotropic junction in the g-C3N4/Au/BiVO4 system. The enhancement in photocatalytic activity is attributed to efficient separation of the photoexcited charges due to the anisotropic junction in the g-C3N4/Au/BiVO4 system.  相似文献   

3.
Metal-free photocatalysts have attracted great attention in hydrogen production under visible light due to their low cost and abundance. Inspired by the structure of chloroplast-granum, here we prepare a new porous nanorod composed of F-doped g-C3N4 ultrathin nanosheet for photocatalytic hydrogen evolution. The obtained g-C3N4 (FCN-PNRs) show layer-by-layer stacked structure for highly efficient light hasting, exhibit F-doping for highly charge separation efficiency, and display porous structure for exposing a large amount of photocatalytic activity sites. These findings have been studied by various characterizations, such as Brunauer-Emmett-Teller, and Photoluminescence. As a result, the hydrogen production performance for the optimized FCN-PNRs photocatalyst reaches 2600 μmol h−1 g−1 under visible light, which is almost 16 times higher than bulk g-C3N4. This study not only reports a new chloroplast-granum-inspired g-C3N4 photocatalyst, but also provides new views to the fabrication and design of nature-inspired metal-free structures for catalysis applications.  相似文献   

4.
Platinum-based alloy materials as effective cocatalysts in improving the performance of photocatalytic H2 production have raised great interest. Herein, a facile strategy of chemical reduction is established to synthesize bimetallic PtNi nanoparticles on 2D g-C3N4 nanosheets with excellent photocatalytic activity. The addition of PtNi nanoparticles can provide new H+ reduction sites and increase more active sites of the material. The synergistic effect between PtNi alloy nanoparticles and 2D g-C3N4 nanosheets can regulate electronic structure, narrow the band, accelerate charge transfer efficiency and inhabit the recombination of photo-induced electron (e) and hole pairs (h+), contributing to the improvement of hydrogen evolution activity. The optimal hydrogen evolution rate of Pt0.6Ni0.4/CN shows higher hydrogen evolution rate (9528 μmol·g−1·h−1), which is 13.1 times than that of pure g-C3N4 nanosheets. Besides, a possible mechanism of photocatalytic hydrogen generation has been brought up according to a series of physical and chemical characterization. This work also provides a potential idea of developing cocatalysts integrating metal alloys with 2D g-C3N4 nanosheets for promoting photocatalytic hydrogen evolution.  相似文献   

5.
Photocatalytic technology for hydrogen evolution from water splitting and pollutant degradation is one of the most sustainable methods. Here, the graphene/g–C3N4–Co composite materials have been prepared by one-pot calcination method. The results show that g-C3N4 grow on the surface of graphene and form a sandwich structure, meanwhile, the introduction of Co increases the active sites, which promotes the photocatalytic performance. The influences of graphene and Co content on photocatalytic activity were also studied by UV–visible spectrophotometry (DRS), photoluminescence spectroscopy (PL), photocurrent, degradation MB, and hydrogen production. The apparent reaction rate constant k of graphene/g–C3N4–Co (3%) is 0.946 h−1, which is 4.90 and 2.18 times faster than g-C3N4 and graphene/g-C3N4, respectively. And the hydrogen production rate of graphene/g–C3N4–Co (3%) (892.3 μmol h−1 g−1) is 3.53 and 1.61 times higher than g-C3N4 and graphene/g-C3N4, respectively.  相似文献   

6.
Two-dimensional (2D) graphitic carbon nitride (g-C3N4) nanosheets, as the promising photocatalyst with fascinating properties, have become a “rising star” in the field of photocatalysis. Although g-C3N4 nanosheets exfoliated from the bulk g-C3N4 powders are extensively emerged, developing a simple synthetic approach is still full of challenge. To this end, here we report a direct polymerization strategy to fabricate the ultrathin g-C3N4 nanosheets, that is only heating treatment of thiourea in air without addition of any template. The photocatalytic activities of as-prepared samples were evaluated by photoreduction of water to hydrogen (H2) using triethanolamine as sacrificial agent and Pt as co-catalyst under visible-light irradiation (λ > 420 nm). As a result, our few-layered g-C3N4 nanosheets with an average thickness of 3.5 nm exhibit a superior visible-light photocatalytic H2 evolution rate (HER) of 1391 μmol g−1 h−1 and a remarkable apparent quantum efficiency of 6.6% at 420 nm. Eventually, the HER of as-fabricated ultrathin g-C3N4 nanosheets is not only much higher than the dicyandiamide-derived g-C3N4 or melamine-derived g-C3N4, but also greater than the thermal-oxidation etched g-C3N4 nanosheets under the same condition.  相似文献   

7.
Excellent light harvest, efficient charge separation and sufficiently exposed surface active sites are crucial for a given photocatalyst to obtain excellent photocatalytic performances. The construction of two-dimensional/two-dimensional (2D/2D) or zero-dimensional/2D (0D/2D) binary heterojunctions is one of the effective ways to address these crucial issues. Herein, a ternary CdSe/WS2/g-C3N4 composite photocatalyst through decorating WS2/g-C3N4 2D/2D nanosheets (NSs) with CdSe quantum dots (QDs) was developed to further increase the light harvest and accelerate the separation and migration of photogenerated electron-hole pairs and thus enhance the solar to hydrogen conversion efficiency. As expected, a remarkably enhanced photocatalytic hydrogen evolution rate of 1.29 mmol g−1 h−1 was obtained for such a specially designed CdSe/WS2/g-C3N4 composite photocatalyst, which was about 3.0, 1.7 and 1.3 times greater than those of the pristine g-C3N4 NSs (0.43 mmol g−1 h−1), WS2/g-C3N4 2D/2D NSs (0.74 mmol g−1 h−1) and CdSe/g-C3N4 0D/2D composites (0.96 mmol g−1 h−1), respectively. The superior photocatalytic performance of the prepared ternary CdSe/WS2/g-C3N4 composite could be mainly attributed to the effective charge separation and migration as well as the suppressed photogenerated charge recombination induced by the constructed type-II/type-II heterojunction at the interfaces between g-C3N4 NSs, CdSe QDs and WS2 NSs. Thus, the developed 0D/2D/2D ternary type-II/type-II heterojunction in this work opens up a new insight in designing novel heterogeneous photocatalysts for highly efficient photocatalytic hydrogen evolution.  相似文献   

8.
Herein, highly efficient and cost effective solar photocatalytic water splitting for hydrogen (H2) generation was achieved by modified g-C3N4. Visible light absorption of g-C3N4 was enhanced by decorating g-C3N4 matrix with silver nanoparticles (Ag). Moreover, incorporation of carbon nanotubes (CNTs) in Ag/g-C3N4 facilitated photocatalytic performance through efficient separation and transfer of photogenerated e-h pairs (charges) in Ag/g-C3N4 that consequently generated very pure and significant H2. Among several tested ratios (wt. %) of Ag/g-C3N4/CNTs, 1.82 (Ag/g-C3N4) and 2.00 (and Ag/g-C3N4/CNTs) were found to be highly efficient that harvested maximum visible-light and produced H2 @1.48 mmol h−1 and 1.78 mmol h−1. We witnessed distinctive role of CNTs as an electron collector and carrier to separate photogenerated e-h pairs to facilitate photocatalysis for H2 generation together with possible utility of Ag and CNTs doped materials with regard to energy transformation.  相似文献   

9.
In this paper, Ag-based g-C3N4 composites have been successfully fabricated through two deferent synthetic methods: (i) a facile and efficient precipitation-calcination strategy (denoted as D–CN–xAg, x represents the dosage of Ag2CO3, the same below), (ii) a calcination method (denoted as Z–CN–xAg). All Ag-based g-C3N4 composites exhibit the enhanced photocatalytic activities under visible-light irradiation. Moreover, the optimal dosage of Ag2CO3 in the D–CN–xAg composite is found to be 5%, the corresponding hydrogen production capacity is 153.33 μmol g−1 h−1, which is 4.6 times higher than that of Z–CN–5%Ag composite. This might be attributed to appropriate content of metallic Ag and more active sites exposed on the surface of D–CN–5%Ag composite. Meanwhile, combining with photoelectrochemical results, it could be inferred that LSPR effect and the intimate interfacial between metallic Ag and g-C3N4 in the system play also important role for the improvement of photocatalytic activity. These results demonstrate that the appropriate loading of metallic Ag originated from Ag2CO3 into g-C3N4 could accelerate the separation and transfer of photogenerated electron-hole pairs, leading to the improvement of photocatalytic activity for hydrogen production from water splitting. Finally, a possible photocatalytic mechanism is proposed.  相似文献   

10.
For the first time, g-C3N4@α-Fe2O3/Co-Pi heterojunctional hollow spheres were successfully fabricated via thermal condensation method followed by solvothermal and photo-deposition treatment, which showed excellent photocatalytical property. Except for the Z-scheme charge transfer between α-Fe2O3 and g-C3N4, the Co-Pi could further reduce the combination of photogenerated electrons and holes as a hole storage agent, resulting in remarkably enhanced visible-light photocatalytic water splitting activity with the H2 production rate of 450 μmol h−1g−1, which is 15.7 times higher than that of g-C3N4. Moreover, the photocatalytic activity of the prepared ternary hollow photocatalysts showed almost no significant weakness after five cycles, which indicated their good performance stability. The as-prepared g-C3N4@α-Fe2O3/Co-Pi also possessed good activity for overall water splitting with the hydrogen production rate reaching 9.8 μmol h−1g−1. This synthesized g-C3N4@α-Fe2O3/Co-Pi composite is expected to be a promising candidate for water splitting.  相似文献   

11.
Ion doping is an effective method to improve the photocatalytic activity of graphitic carbon nitride (g-C3N4) by providing a photocarriers transfer channel. But limited by the bonds in heptazine rings, photoelectrons are still trapped in the structure. Therefore, both potassium ions and nitrogen defects were successfully introduced into g-C3N4 by high temperature calcination to accelerate the charges transfer between both interlayers and intralayer of g-C3N4. The results showed that the hydrogen production rate of g-C3N4 modified simultaneously by nitrogen defects and potassium ions reaches 1722.4 μmol·g−1·h−1, which is 8 times that of pristine g-C3N4. Based on various characterization techniques and DFT calculations, we attributed the enhanced photocatalytic hydrogen evolution to the improved light adsorption, more delocalized HOMO-LUMO, and stronger interlayer interactions. This work will provide a promising way to enhance photocatalytic hydrogen evolution of g-C3N4 and a possible mechanism was proposed.  相似文献   

12.
Ceria dioxide supported on graphitic carbon nitride (CeO2/g-C3N4) composites were facilely synthesized to be application for photocatalytic hydrogen (H2) generation in this present work. The physical and chemical properties of CeO2/g-C3N4 nanocomposites were determined via a series of characterizations. The CeO2/g-C3N4 composites prepared by facile thermal annealing and rotation-evaporation method exhibit excellent photocatalytic H2 evolution with visible-light illumination. The best hydrogen generation rate of CeO2/g-C3N4 composite with 1.5 wt% Pt is 0.83 mmol h−1 g−1, which is almost same as that of composite with 3 wt% Pt prepared by simple physical mixing method. The significantly developed photocatalytic activity of CeO2/g-C3N4 composite is majorly ascribed to the stronger interfacial effects with the more visible-light absorbance and faster electron transfer. This work reveals that construction of the CeO2/g-C3N4 composite with high disperse and close knit by the facile thermal annealing and rotation-evaporation method could be an effective method to achieve excellent photocatalytic hydrogen evolution performance.  相似文献   

13.
g-C3N4 has shown great potentials in photocatalytic water splitting to produce hydrogen. Herein, we successfully synthesized g-C3N4 nanosheets via exfoliating bulk g-C3N4. And different metal nanoparticles were photo-deposited onto the surface of g-C3N4 nanosheets. The photocatalytic H2 production activity of g-C3N4 nanosheets increased from 0 to 11.2 μmol/h/gcat. The Pt loaded g-C3N4 nanosheets manifested the highest H2 production activity with a rate of 589.4 μmol/h/gcat. In addition, the hydrogen evolution rate was further enhanced with addition of external bias to fabricate a photoelectrocatalytic (PEC) system. And the maximum hydrogen production rate (23.1 mmol/h/m2) was obtained at a voltage of 0.6 V (vs. Ag/AgCl). The enhancement in H2 production may be due to the following reasons: (1) Two-dimensional atomic flakes is beneficial to increase the specific surface area of g-C3N4, enhance the mobility of carriers, and improve the energy band structure, (2) Pt nanoparticles play an important role in g-C3N4 electron transport, (3) the g-C3N4 nanosheets loaded with Pt nanoparticles exhibited significant enhancement in photoelectrocatalytic performance, which may be attributed to its enhanced electronic conductivity and photoelectrochemical surface area, (4) Pt inhibited the recombination of photogenerated carriers and significantly improved the photocatalytic performance. The enhancement mechanism was deeply discussed and explained in this work.  相似文献   

14.
Bio-mimetic C-doped graphitic carbon nitride (g-C3N4) with mesoporous microtubular structure has been prepared by a simple chemical wet bio-template impregnation approach (direct impregnation and hydrothermal impregnation) using urea as a precursor and kapok fibre as bio-template and in-situ carbon dopant. Our finding indicated that the hydrothermal impregnation had induced more in-situ C-doping in g-C3N4 as compared to the direct impregnation approach. The introduction of in-situ C doping in the g-C3N4 and the mesoporous microtubular structure remarkably enhanced light-harvesting capability up to near infrared regions. The photocurrent measurement and electrochemical impedance spectroscopy (EIS) analysis suggested that the bio-template C-doped g-C3N4 exhibits a superior photoinduced electron-hole pairs separation efficiency due to C doping and mesoporous microtubular structure significantly promotes excellent conductivity and electron redistribution in the sample. C-doped graphitic carbon nitride sample prepared by the hydrothermal (HB/g-C3N4) approach exhibits excellent photocatalytic hydrogen production with an H2 production rate of 216.8 μmol h−1 g−1 which was a 1.3 and 2.9 improvement over C-doped graphitic carbon nitride prepared by direct impregnation (DB/g-C3N4) and pristine g-C3N4, respectively. This study provides new insights into the development of low-cost and sustainable photocatalysts for photocatalytic hydrogen production.  相似文献   

15.
The photocatalytic hydrogen evolution performance of g-C3N4 was enhanced via the hybridization with montmorillonite (MMT) and using NiCoP as cocatalyst. The highest hydrogen-evolution rate from water splitting under visible-light irradiation observed over MMT/g-C3N4/15%NiCoP was 12.50 mmol g−1 h−1 under 1.0 mmol L−1 of Eosin Y-sensitization at pH of 11, which was ∼26.0 and 1.6 times higher than that of MMT/g-C3N4 (0.48 mmol g−1 h−1) and g-C3N4/15%NiCoP (7.69 mmol g−1 h−1). The apparent quantum yield at 420 nm reached 40.3%. The remarkably improved photocatalytic activity can be ascribed to the increased dispersion of g-C3N4 layers, staggered conduction band potentials between g-C3N4 and NiCoP, as well as the electrostatic repulsion originated from negatively charged MMT. This work demonstrates that MMT can be an outstanding support for the deposition of catalytically active components for photocatalytic hydrogen production.  相似文献   

16.
Construction of heterostructured photocatalysts is a feasible method for improving hydrogen production from water splitting because of its good charge transport efficiency. Herein, we coupled the Ti-MOFs (TiATA) with metal-free graphitic carbon nitride (g-C3N4) to synthesize composites, g-C3N4@TiATA, in which a heterostructure was formed between g-C3N4 and TiATA. The establishment of heterojunctions not only broadens the light absorption range of g-C3N4@TiATA (490 nm) by contrast with g-C3N4 (456 nm), but also greatly accelerates charge migration. Photocatalytic studies present that the construction of heterostructure steering the charges flow from g-C3N4 to TiATA and then delivery to the cocatalyst of Pt nanoparticles, exhibiting an impressively photocatalytic hydrogen production rate (265.8 μmol·h−1) in assistance of 300 W Xenon lamp, which is about 3.4 times as much as g-C3N4/Pt.  相似文献   

17.
Graphitic carbon nitride (g-C3N4) has been well-known as an appealing semiconducting material for photocatalytic hydrogen production despite its restricted active sites and poor electronic properties. In this work, exfoliated g-C3N4 nanosheets were synthesised by chemical treatment of the bulk graphitic carbon nitride (gCN) and the nanosheets were further doped with CdO. The photocatalysts produced were extensively characterized by diverse analysis including XRD, BET, XPS, TEM, FESEM, UV-Vis spectroscopy and PL analysis. The BET surface area of CdO/exfoliated g-C3N4, 40.1 m2 g−1 was doubled in comparison to the exfoliated g-C3N4. Numerous electrochemical analyses such as Mott-Schottky, linear weep voltammetry and chronoamperometry were also performed in a standard photoelectrochemical system with three-electrode cell. The hydrothermally synthesised CdO/exfoliated g-C3N4 resulted higher amount of hydrogen evolution (145 μmol/g) for the photoreforming of aqueous formaldehyde than the CdO (20 μmol/g), bulk gCN (58 μmol/g) and exfoliated g-C3N4 (87 μmol/g). The excellent hydrogen production rate using CdO/exfoliated g-C3N4 nanocomposite could be ascribed by higher number of active sites as well as shorter path of the charge carries to the reaction surface. The anticipated Z-Scheme mechanism has demonstrated a synergistic impact between the CdO and exfoliated g-C3N4 where the organic compounds acting as hole scavenger as well as contribute protons, H+ for the effective hydrogen production. Thus, it is clearly confirmed that the newly formulated CdO/exfoliated g-C3N4 has an outstanding potentiality for environmental remediation and conversion sectors.  相似文献   

18.
Graphite-like carbon nitride (g-C3N4) has been regarded as a promising photocatalyst for solar-to-chemical conversion. Nevertheless, the narrow absorption of light extremely limited its photocatalytic performance under near-infrared (NIR) irradiation. Herein, the Cu7.2S4 with outstanding NIR absorption was successfully introduced to g-C3N4 nanosheets through a simple in-situ growth procedure. As expected, the constructed Cu7.2S4/g-C3N4 (CSCN) photocatalysts exhibit superior H2 production activity of 82 μmol g−1 h−1 under NIR light irradiation (λ > 800 nm), which outperforms currently reported g–C3N4–based NIR-driven H2 production systems. Especially, the optimal sample CSCN-5 displays a robust activity of 66 μmol g−1 h−1 at λ = 850 nm monochromatic light irradiation. The excellent photocatalytic performance is linked to the extended optical absorption as well as the efficient separation efficiency of photoinduced carriers, which are evidenced by the UV-visible absorption spectroscopy and photoelectrochemical test. This work provides an effective approach for constructing a Cu7.2S4/g-C3N4 photocatalytic system for the transformation of NIR solar energy into hydrogen.  相似文献   

19.
TiO2-x/g-C3N4/CdS ternary heterojunctions are fabricated through thermal polymerization-chemical bath deposition combined with in-situ solid-state chemical reduction approach. The prepared materials are characterized by X-ray diffraction, Fourier transform infrared spectra, scanning electron microscopy, transmission electron microscopy, nitrogen adsorption-desorption, and X-ray photoelectron spectroscopy. The results show that the ternary heterojunctions are formed successfully and CdS quantum dots (QDs) and TiO2 are anchored on surface of g-C3N4 nanosheets simultaneously. The visible-light-driven photocatalytic degradation ratio of Bisphenol A and hydrogen production rate are up to 95% and ∼254.8 μmol h−1, respectively, which are several times higher than that of pristine TiO2. The excellent visible-light-driven photocatalytic activity can be ascribed to the synergistic effect of TiO2−x, g-C3N4 and CdS QDs which extend the photoresponse to visible light region and favor the spatial separation of photogenerated charge carriers.  相似文献   

20.
Solar-light responsive platinum/graphite-like carbon nitride/strontium titanate (Pt/g-C3N4/SrTiO3) with excellent charge separation was synthesized via thermal treatment process. A photocatalytic hydrogen production rate of 552 μmol/h/g was achieved under simulated sunlight irradiation for the Pt/(g-C3N4/SrTiO3) catalyst with 5 v/v% triethanolamine (TEOA) as a sacrificial agent. The hydrogen production rate of Pt/g-C3N4/SrTiO3 prepared via different synthetic sequences decreased in the following order: Pt/(g-C3N4/SrTiO3) > (Pt/g-C3N4)/SrTiO3 > g-C3N4/(Pt/SrTiO3). The mechanisms of electron transfer in the different synthetic sequences of Pt/g-C3N4/SrTiO3 were investigated. The electron transfer pathway of Pt/(g-C3N4/SrTiO3) was as follows: (1) g-C3N4→SrTiO3→Pt, (2) g-C3N4→Pt, (3) SrTiO3→Pt, and (4) g-C3N4→SrTiO3, leading to optimal charge separation and H+ ion reduction.  相似文献   

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