首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
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   

2.
Engineering surface-active facets of metal cocatalysts is one of the most widely explored strategies to develop advanced photocatalysts and promote photocatalytic solar energy conversion. Here, the surface-active facets of Pd nanocrystals in Pd/g-C3N4 photocatalyst was related to the injection flow rate of PdCl2. When PdCl2 was injected at a low flow rate of 7.5 mL/h (7.5-Pd/g-C3N4), the Pd nanocrystals were uniformly dispersed onto the g-C3N4 with exposed low-index {100} and {111} surface-active facets. However, increasing the injection flow rate to 150 mL/h (150-Pd/g-C3N4) formed Pd nanocrystals where only the {100} surface-active facet was exposed. Under visible light irradiation, the 7.5-Pd/g-C3N4 nanocomposite exhibited excellent water splitting activity for hydrogen production (7.61 mmol g−1 h−1), which was significantly better than with the 150-Pd/g-C3N4 nanocomposite (3.3 mmol g−1 h−1). Theoretical calculations and experimental results confirm the importance of the {111} surface-active facets in the 7.5-Pd/g-C3N4 nanocomposite for promoting photocatalytic activity.  相似文献   

3.
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   

4.
Increased charge transfer and light absorption as well as large specific surface area are effective ways to improve the catalytic efficiency of photocatalysts. In this paper, barbituric acid, urea and thiourea were separately freeze-dried to form a homogeneous precursor with melamine, followed by thermal polymerization at 750 °C, g-C3N4 was doped successfully with C, N and S. Among them, C-doped g-C3N4 revealed well photocatalytic hydrogen production which reached to 2.45 mmol g−1 h−1. N-doped g-C3N4 exhibited enhanced photocatalytic degradation properties for organic dye (RhB) which is completely degraded within 8 min while the performance S-doped sample is not satisfied. The introduction of C resulted in planarized sample which has a larger specific surface area and provides more active sites. N doping makes the valence band position moving in the direction of high energy. Thus, holes have stronger oxidizing ability. Accordingly, the effect of C and N ratios in g-C3N4 photocatalysis was fully discussed for more comprehensive understanding of g-C3N4.  相似文献   

5.
Controlled integration of metal-based sulfides with phosphides possessing strong coupling effects is a promising way to accelerate electron transfer by modulating the electronic structures of the host species. In this work, a c-doped Ni3S4/Ni2P (C@Ni3S4/Ni2P) hybrid co-catalyst produced by in situ sulfuration and phosphidation of Ni-MOF was decorated on g-C3N4 and subsequently used for photocatalytic H2 evolution under visible-light irradiation. Among the prepared composites tested herein, the optimized g-C3N4/C@Ni3S4/Ni2P-30 composite showed the highest H2 evolution rate (14.49 mmol g−1 h−1) with 1.0 mmol L−1 of Eosin Y (EY)-sensitization, which is 10 times higher than that of pristine g-C3N4 (1.33 mmol g−1 h−1). The enhanced photocatalytic activity of this composite can be attributed to: (i) electronic interactions between Ni2P and Ni3S4 (which synergistically increased the electron transfer rate) and (ii) staggered band alignment of excited-stated EY, g-C3N4, Ni3S4, and Ni2P. This work may provide some perspectives for utilization of MOF-derived hybrid co-catalysts as substitutes of noble metals for effective photocatalytic H2 evolution.  相似文献   

6.
Well dispersed CdS quantum dots were successfully grown in-situ on g-C3N4 nanosheets through a solvothermal method involving dimethyl sulfoxide. The resultant CdS–C3N4 nanocomposites exhibit remarkably higher efficiency for photocatalytic hydrogen evolution under visible light irradiation as compared to pure g-C3N4. The optimal composite with 12 wt% CdS showed a hydrogen evolution rate of 4.494 mmol h−1 g−1, which is more than 115 times higher than that of pure g-C3N4. The enhanced photocatalytic activity induced by the in-situ grown CdS quantum dots is attributed to the interfacial transfer of photogenerated electrons and holes between g-C3N4 and CdS, which leads to effective charge separation on both parts.  相似文献   

7.
Here we report a 2D-2D heterostructure of g-C3N4/UMOFNs photocatalysts via mechanical grinding two kinds of two-dimensional nanosheets of g-C3N4 nanosheets and UMOFNs, which exhibits enhanced H2 evolution from water with simulated solar irradiation. g-C3N4 nanosheets are in close contact with UMOFNs, and there is a certain interaction between them, showing the effect of superimposition on the two-dimensional layer. The 2D-2D heterostructure offers a maximal photocatalytic hydrogen production activity of 1909.02 μmol g−1 h−1 with 3 wt% of UMOFNs, which is 3-fold higher than that of g-C3N4 nanosheets (628.76 μmol g−1 h−1) and 15-flod higher than that of bulk g-C3N4 (124.30 μmol g−1 h−1). The significant increasement of photocatalysis is due to 2D-2D heterostructure possessing a short charge transfer distance and large contact area between g-C3N4 and UMOFNs. The highly dispersed NiO, CoO and π-π bonds in UMOFNs of 2D-2D structure also promote charge transfer and enhance the photocatalytic activity.  相似文献   

8.
Facilitating the separation of photoexcited electron-hole pairs and enhancing the migration of photogenerated carriers are essential in photocatalytic reaction. CoS/g-C3N4/NiS ternary photocatalyst was prepared by hydrothermal and physical stirring methods. The optimized ternary composite achieved a hydrogen yield of 1.93 mmol g?1 h?1, 12.8 times that of bare g-C3N4, with an AQE of 16.4% at 420 nm. The enhanced photocatalytic activity of CoS/g-C3N4/NiS was mainly ascribed to the synergistic interaction between the Z-scheme heterojunction constructed by CoS and g-C3N4 and the NiS co-catalyst featuring a large amount of hydrogen precipitation sites, which realized the efficient separation and migration of photogenerated carriers. In addition, the CoS/g-C3N4/NiS heterojunction-co-catalyst system exhibited excellent photocatalytic stability and recyclability.  相似文献   

9.
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   

10.
Novel PdAg bimetallic alloy nanoparticle modified graphitic carbon nitride (g-C3N4) nanosheet was designed and prepared by an in situ chemical reduction procedure. By optimizing the loading content of the PdAg alloy NPs, the PdAg/g-C3N4 composite photocatalyst showed a champion photocatalytic hydrogen generation rate of 3.43 mmol h−1 g−1, and the apparent quantum yield (AQY) was determined to be 8.43% at 420 nm. Moreover, the photoluminescence and photoelectrochemical experimental results suggest that a higher separation efficiency of photo-induced charge carriers (e- and h+) was obtained after loading PdAg alloy NPs on g-C3N4. The experimental outcomes indicate that there is a synergistic effect formed between PdAg and g-C3N4, which could significantly promote the charge transfer photo-induced charge carriers in the hybrid sample. A reasonable catalytic mechanism for the enhanced photocatalytic performance of the composite photocatalyst was proposed and verified by TRPL measurement, which could be taken as a guidance for the development of novel high performance catalytic system.  相似文献   

11.
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   

12.
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   

13.
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   

14.
The practical applications of graphitic carbon nitride (g-C3N4) for photocatalytic hydrogen evolution is strictly hindered by the low surface area, poor light harvesting capability and detrimental recombination of photoexcited charge carriers. Herein, using melamine as precursor and metal hydride (i.e., CaH2) as active agent, we facilely incorporate various types of defects (i.e., nitrogen (N) vacancies (VN), cyano groups (CN) and surface absorbed oxygen species(Oabs)) into g-C3N4 within a single step. The as-prepared material (denoted as MM-H) exhibits narrowed bandgap, promoted photoexcited electron-hole separation rate and facilitated charge transfer kinetics with enlarged BET surface area and massive porosity. As a result, a prominently enhanced photocatalytic H2 productivity efficiency (1305.9 μmol h−1g−1) is shown on MM-H. This performance is better than that of g-C3N4 with CaH2 post-treatment (617.3 μmol h−1g−1) and raw bulk-C3N4 (178.2 μmol h−1g−1). This work opens up a new dimension for designing high performance g–C3N4–based catalysts targeting various photocatalytic processes.  相似文献   

15.
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   

16.
The hybrid 1D branched TiO2 loaded with g-C3N4 QDs was successfully fabricated that plays a significant role in photocatalysis. The 1D branched TiO2 prepared by electrospinning followed by alkali-hydrothermal process, and g-C3N4 QDs were grafted over it by a chemical vapor deposition method. The composite display enhancement in photocatalytic hydrogen evolution is about 10.57 mmol. g−1.h−1 in comparison to the g-C3N4 sample that only produces 0.32 mmol. g−1.h−1 while the HBTiO2 sample evolved a negligible amount of hydrogen under visible light. The composite sample shows quantum efficiency for HER at 420 nm light is 18.6% that is much higher than the other two samples. The specific surface area of the composite sample is 92.39 m2g-1 that is about 13 times more than bulk g-C3N4. The bandgap of HBTiO2/g-C3N4 QDs, g-C3N4, and HBTiO2 samples calculated as 2.71 eV, 2.67eV, and 3.24eV, respectively. The TRPL spectra imply that the duration of the lifetime of composite becomes longer which effectually overwhelm the electron-hole recombination. The 1D branched TiO2 fiber reduces the charge recombination by fast transfer of electron while g-C3N4 QDs facilitate the visible light absorption by improving the optical properties. The formation of the type II heterostructure system remarkably promotes the separation and transfer of electron holes and facilitates the photo-reduction reaction.  相似文献   

17.
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   

18.
In this study, B-doped g-C3N4 nanosheets (BCN) were prepared using a thermal-oxidative etching method, resulting in a semiconductor with a large specific surface area. The B-doping enhances the light absorption of graphitic carbon nitride(g-C3N4) and improves the photogenerated carrier lifetime. The optimal B-containing amount resuled in a hydrogen production rate of 1297 μmol g−1 h−1 for g-C3N4 nanosheets. Furthermore, zeolitic imidazolate framework (ZIF)67/BCN heterostructures were successfully obtained through simple mechanical grinding approaches. The BCN provided abundant active sites and contributed to excellent encapsulation on the surface of ZIF67. The obtained ZIF67/BCN photocatalyst displayed an H2 evolution rate of 3392 μmol g−1 h−1, attributed to forming type-II heterojunctions between ZIF67 and BCN. Moreover, the BCN exhibited a higher conduction band (CB) potential with ZIF67 than CN, resulting in more efficient light-driven charge separation between ZIF67 and BCN and enhanced photocatalytic performance. This work provides a meaningful reference for improving the activity of g-C3N4 photocatalysts.  相似文献   

19.
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   

20.
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   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号