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1.
Structure and interface control of heterojunction is usually a challenging issue to improve the photocatalytic performance. Herein, a new 3D/2D CoCO3/g-C3N4 heterojunction is assembled by embedding hexahedral CoCO3 on g-C3N4 nanosheets. The unique step-like hierarchical structure of CoCO3, the formed built-in electric field and Z-scheme charge transfer behavior at the interface jointly drive the high-efficient separation of photogenerated carriers to boost the photocatalytic H2 production. It achieves the optimal H2 production rate that is almost 2.6 times than g-C3N4, apparent quantum efficiency (AQE) of 10.1% at 400 nm and continuous running of 60 h over the 3D/2D CoCO3/g-C3N4 heterojunction. This work endows a fresh structural control strategy for the fabrication of 3D/2D Z-scheme heterojunction to improve the photocatalytic H2 production performance.  相似文献   

2.
Development of low cost and efficient non-noble-metal cocatalyst is still a hot topic to improve the activity of g-C3N4 in photocatalytic water splitting to produce H2. As a potential cocatalyst in photocatalytic application, transition metal phosphides (TMPs) have been proved to greatly enhance the photocatalytic H2 evolution performance comparable to noble metal Pt. Modifying TMPs by incorporation of hetero-metal has also been reported as an effective strategy for their electronic structure regulation and optimizing the intermediates absorption energy, however, which is rarely reported in the field of photocatalysis. Herein, the 0D/2D heterojunction is constructed by high-dispersity Mo-doped Ni2P nanodots supported on g-C3N4 nanosheets, which exhibits the significantly improved photocatalytic H2 evolution performance compared with that of Ni2P/g-C3N4 and Pt/g-C3N4. Specifically, the optimal H2 evolution rate reaches 67.6 μmol h−1 over Mo–Ni2P/g-C3N4 sample, which is 6.0 and 2.4 times higher than those of Pt/g-C3N4 and Ni2P/g-C3N4, respectively. The fascinating result mainly stems from the improved separation efficiency of charge carriers and more effective electron donating reaction sites resulted from the electronic structure adjustment through doping Mo element into Ni2P as cocatalyst. This work provides a valid evidence for the modification of cocatalyst to realize high H2 evolution performance, opening up new opportunities and possibilities for the application of TMPs in the photocatalytic field.  相似文献   

3.
Fabricating 0D/2D heterojunctions is considered to be an efficient mean to improve the photocatalytic activity of g-C3N4, whereas their applications are usually restricted by complex preparation process. Here, the 0D/2D SnO2/g-C3N4 heterojunction photocatalyst is prepared by a simple one-step polymerization strategy, in which SnO2 nanodots in-situ grow on the surface of g-C3N4 nanosheets. It shows the outstanding photocatalytic H2 production activity relative to g-C3N4 under the visible light, which is due to the formation of 0D/2D heterojunction significantly contributing to the separation of photogenerated charge carriers. In particular, the H2 production rate over the optimal SnO2/g–C3N4–1 sample is 1389.2 μmol h−1 g−1, which is 6.06 times higher than that of g-C3N4 (230.8 μmol h−1 g−1). Meanwhile, the AQE value of H2 production over the SnO2/g–C3N4–1 sample reaches up to a maximum of 4.5% at 420 nm. This work develops a simple approach to design and fabricate g–C3N4–based 0D/2D heterojunctions for the high-efficiency H2 production from water splitting.  相似文献   

4.
ZnCr layered double hydroxides (ZnCr LDH) nanosheets modified graphitic carbon nitride (g-C3N4) nanohybrids were fabricated via a self-assembly procedure through electrostatic interaction between these two components. Such 2D-2D inorganic-organic hybrid material was employed for photocatalytic hydrogen production under visible light for the first time. The physical and photophysical properties of the hybrid nanocomposites were investigated to reveal the effect of ZnCr LDH nanosheets on the photocatalytic activities of g-C3N4. It was found that 1 wt% ZnCr LDH nanosheets modified g-C3N4 was optimal for the formation of intimate interfacial contact. The visible light photocatalytic H2 production activity over g-C3N4 was enhanced about 2.8 times after ZnCr LDH nanosheets modification. The significant enhancement in photocatalytic performance for ZnCr LDH/g-C3N4 heterojunction should be attributed to the promoted charge transfer and separation efficiency, resulting from the intimate interfacial contact and Type II band alignment between ZnCr LDH and g-C3N4.  相似文献   

5.
A 2D g-C3N4(pPCN)/rGO heterojunction for photocatalytic hydrogen production is fabricated by a facile dissolution strategy facilitated by H2SO4. The bulk g-C3N4 (CN) can be directly exfoliated into ultrathin protonated g-C3N4 (PCN) nanosheets under the assistance of H2SO4, and PCN can be further modified by rGO in a dissolved state under the electrostatic self-assembly process. The nanocomposite exhibits a large surface area (146.47 m2/g) and intimate contact interfaces between pPCN and rGO due to the specific synthesis method. Based on the DRS, PL and photoelectrochemical analyses, the introduction of rGO can greatly improve the light absorption and photogenerated charge carrier separation and transfer of g-C3N4. The optimal pPCN/2 wt% rGO nanocomposite shows an efficient photocatalytic H2 evolution rate of 715 μmol g?1 h?1 under visible light irradiation, which is 2.6 and 13 times higher than those obtained on pPCN and CN. In addition, a photocatalytic mechanism over a 2D pPCN/rGO heterojunction is proposed. This work offers a new effective strategy for fascinating gC3N4based nanocomposites with promising hydrogen generation.  相似文献   

6.
The effective separation of photogenerated charge carriers, their transport and interfacial contact is of great significance for excellent performance of semiconductor based photocatalysts. Herein, we report the fabrication of two dimensional (2D) nanosheets heterojunction comprising of N-doped ZnO nanosheets loaded over graphitic carbon nitride (g-C3N4) nanosheets for enhanced photocatalytic hydrogen evolution. The prepared 2D-2D heterojunctions with varying amount of g-C3N4 nanosheets have been characterized by x-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and x-ray photoelectron spectroscopy (XPS) techniques. The optimized heterojunction photocatalyst with 30 wt% of g-C3N4 nanosheets (NZCN30) exhibit hydrogen evolution rate of 18836 μmol h?1 gcat?1 in presence of Na2S and Na2SO3 as sacrificial agents under simulated solar light irradiation. The enhanced photocatalytic performance of NZCN30 heterojunction has been supported well by photoluminescence and photoelectrochemical investigations, which shows the minimum recombination rate and high photoinduced current density, respectively. In addition, the existence of 2D-2D interfacial contact plays a major role in enhanced H2 evolution by high face-to-face contact surface area for separation of photogenerated charge carriers in space which facilitate their transfer for H2 generation. This work paves way for the development of 2D-2D heterojunctions for diverse applications.  相似文献   

7.
The weaker van der Waals force between layers inhibits the interlayer electron migration, which greatly limiting the enhancement of the photocatalytic activity over graphitic carbon nitride (g-C3N4). Herein, the metal-free sulfur-doped 2D/3D van der Waals (vdW) homojunction (2D/3D CNSCN) that containing 2D sulfur-doped g-C3N4 nanosheets (CNS) and 3D g-C3N4 flower-like hierarchical structure (CN) was fabricated. Thanks to the cooperative effect of 2D-3D structural and good compatibility between CNS and CN, an in situ formed 2D/3D vdW homojunction served as the driving force for promoting charge carrier separation and transfer. The optimal photocatalytic H2 evolution of 2D/3D CNSCN reached up to 2196 μmol h?1g?1, which was 4.1 and 3.2 times higher than that of CN and CNS, respectively. 10 mg of the 2D/3D CNSCN photocatalyst was able to totally remove of rhodamine B (RhB) solution in less than 80 min under the visible light. This study provides new opportunities to construct novel 2D/3D mixed-dimensional vdW homojunction, and broad interest in vdW homojunction research for the applications in energy conversion and environmental protection field.  相似文献   

8.
Constructing 2D/2D heterojunction photocatalysts has attracted great attentions due to their inherent advantages such as larger interfacial contact areas, short transfer distance of charges and abundant reaction active sites. Herein, 2D/2D CoP/CdS heterojunctions were successfully fabricated and employed in photocatalytic H2 evolution using lactic acid as sacrificial reagents. The multiple characteristic techniques were adopted to investigate the crystalline phases, morphologies, optical properties and textual structures of heterojunctions. It was found that integrating 2D CoP nanosheets as cocatalysts with 2D CdS nanosheets by Co–S chemical bonds would significantly boost the photocatalytic H2 evolution performances, and the 7 wt% 2D/2D CoP/CdS heterojunction possessed the maximal H2 evolution rate of 92.54 mmol g?1 h?1, approximately 31 times higher than that of bare 2D CdS nanosheets. Photoelectrochemical, steady photoluminescence (PL) and time-resolved photoluminescence (TRPL) measurements indicated that there existed an effective charge separation and migration over 2D/2D CoP/CdS heterojunction, which then markedly lengthened the photoinduced electrons average lifetimes, retarded the recombination of charge carriers, and caused the dramatically boosted photocatalytic H2 evolution activity. Moreover, the density functional theory (DFT) calculation further corroborated that the efficient charge transfer occurred at the interfaces of CoP/CdS heterojunction. This present research puts forward a promising strategy to engineer the 2D/2D heterojunction photocatalysts endowed with an appealing photocatalytic H2 evolution performance.  相似文献   

9.
Although graphitic carbon nitride (g-C3N4) is widely used for photocatalytic hydrogen production, its practical application is restricted by the high recombination rate of photoinduced electron-hole pairs and limited active sites. In this work, holey ultrathin g-C3N4 nanosheets (HCN NSs) with rich active sites are prepared, followed by the growth of 1T-MoS2 NSs on their surfaces to construct 2D/2D 1T-MoS2/HCN heterostructure. Due to the high surface area and abundant hydrogen active sites of the hybrid, large and intimate 2D nanointerface between MoS2 and HCN, hydrogen ion adsorption and charge separation/transport ability are greatly enhanced. As a result, 1T-MoS2/HCN-4 with the optimal 1T-MoS2 content of 8 wt% displays the highest H2 production rate of 2724.2 μmol?1 h?1 g?1 under simulated solar light illumination with apparent quantum efficiency of 8.1% (λ = 370 nm). Moreover, the 1T-MoS2/HCN-4 hybrid manifests improved stability after a long-time test. This study opens the door to design highly-efficient g-C3N4 based 2D/2D heterostructures for photocatalytic H2 production.  相似文献   

10.
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   

11.
Graphitic carbon nitride (g-C3N4) is one of the promising two-dimensional metal-free photocatalysts for solar water splitting. Regrettably, the fast electron-hole pair recombination of g-C3N4 reduces their photocatalytic water splitting efficiency. In this work, we have synthesized the CuO/g-C3N4 heterojunction via wet impregnation followed by a calcination method for photocatalytic H2 production. The formation of CuO/g-C3N4 heterojunction was confirmed by XRD, UV–vis and PL studies. Notably, the formation of heterojunction not only improved the optical absorption towards visible region and also enhanced the carrier generation and separation as confirmed by PL and photocurrent studies. The photocatalytic H2 production results revealed that CuO/g-C3N4 photocatalyst demonstrated the increased photocatalytic H2 production rate than bare g-C3N4. The maximum H2 production rate was obtained with 4 wt % CuO loaded g-C3N4 photocatalyst. Importantly, the rate of H2 production was further improved by introducing simple redox couple Co2+/Co3+. Addition of Co2+ during photocatalytic H2 production shuttled the photogenerated holes by a reversible conversion of Co2+ to Co3+ with accomplishing water oxidation. The effective shuttling of photogenerated holes decreased the election-hole pair recombination and thereby enhancing the photocatalytic H2 production rate. It is worth to mention that the addition of Co2+ with 4 wt % CuO/g-C3N4 photocatalyst showed ∼7.5 and ∼2.0 folds enhanced photocatalytic H2 production rate than bare g-C3N4/Co2+ and CuO/g-C3N4 photocatalysts. Thus, we strongly believe that the present simple redox couple mediated charge carrier separation without using noble metals may provide a new idea to reduce the recombination rate.  相似文献   

12.
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   

13.
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   

14.
In this paper, a novel Au/g-C3N4/ZnIn2S4 plasma photocatalyst heterojunction composite with 3D hierarchical microarchitecture has been successfully constructed by integrating Au/g-C3N4 plasmonic photocatalyst composite with 3D ZnIn2S4 nanosheet through a simple hydrothermal process. The Au nanoparticles were firstly anchored on the surface of pristine g-C3N4 material to get Au/g-C3N4 plasmonic photocatalyst. Ascribing to the surface plasmon resonance of Au nanoparticles, the obtained Au/g-C3N4 plasmonic photocatalyst shows a significant improved photocatalytic activity toward hydrogen production from water with visible light response comparing with pristine g-C3N4. Further combining Au/g-C3N4 plasmonic photocatalyst with 3D ZnIn2S4 nanosheet to construct a heterojunction composite. Owing to the synergistic effect of the surface plasmon resonance of Au nanoparticles in Au/g-C3N4 and the heterojunction structure in the interface of Au/g-C3N4 and ZnIn2S4, the prepared Au/g-C3N4/ZnIn2S4 plasma photocatalyst heterojunction composite shows an excellent photocatalytic activity toward hydrogen production from water with visible light response, which is around 7.0 and 6.3 times higher than that of the pristine C3N4 and Znln2S4 nanosheet, respectively. The present work might provide some insights for exploring other efficient heterojunction photocatalysts with excellent properties.  相似文献   

15.
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   

16.
WO3/g-C3N4 two-dimensional (2D) composite photocatalysts were prepared through a simple hydrothermal method followed by a post thermal treatment. The H2 generation activity of these photocatalysts in the visible light was evaluated. The photocatalysts were characterized by X-ray powder diffraction, Fourier transform infrared spectra, transmission electron microscopy and UV–vis diffuse reflectance spectroscopy et al. These results show that the orthorhombic-phase WO3 nanoparticles with a grain size from 5 to 80 nm were successfully anchored on g-C3N4 nanosheets surface with intimate contact. Furthermore, the charge separation mechanisms of photo-generated charge carriers of the 2D WO3/g-C3N4 photocatalysts were further studied by photoelectrochemical response and electrochemical impedance spectroscopy. The result shows that the 2D WO3/g-C3N4 photocatalyst with 10 wt% WO3 possesses the maximum photocatalytic performance for H2 generation, as high as of 1853 μmol h?1 g?1, which is about 6.5 times higher than that of bare g-C3N4, indicating the fast injection of interface interaction between 2D g-C3N4 and WO3. The increased photocatalytic performance of the composite photocatalyst can be attributed to the enhanced absorption of visible light, the higher photo-generated electrons and holes separation efficiency and low recombination rate of electrons and holes generated by photoexcitation.  相似文献   

17.
Photocatalytic H2 generation has been believed to be a hopeful technology to deal with the current energy shortage issue. Among multifarious photocatalysts, graphitic carbon nitride (g-C3N4) has acquired enormous interests in virtue of its numerous advantages, such as peculiar physicochemical stability, favorable energy band structure and easy preparation. However, the insufficient light response range, low specific surface area, and inferior charge separation efficiency make its photocatalytic activity still unsatisfactory. In this work, the thermal exfoliation method was taken to prepare the thin g-C3N4 nanosheets with significantly improved specific surface area, which can afford more reaction sites and shorten the charge migration distance. Moreover, phosphorus (P) doping in g-C3N4 nanosheets can greatly expand its light absorption, improve the conductivity and charge-transfer capability. Due to the synergistic effect of these two strategies, the optimal H2 generation performance of P-doped g-C3N4 nanosheets came up to 1146.8 μmol g?1 h?1, which improved 15, 2.94 and 2.62 times compared to those of original bulk g-C3N4, thermally exfoliated g-C3N4 and P-doped bulk g-C3N4, respectively. The synergistic effect will inspire the design of other photocatalytic systems to achieve the efficient photocatalytic H2 generation activity.  相似文献   

18.
Novel carbon dots (CDs)/graphitic carbon nitride (g-C3N4) hybrids were fabricated via an in situ thermal polymerization of the precursors, urea and glucose. This heterojunction catalyst exhibited enhanced photocatalytic H2 evolution activity under visible-light (λ > 420). A sample of CDs/g-C3N4 hybrids, CN/G0.5, which was prepared from 0.5 mg of glucose in 6.0 g of urea (8.3 × 10?3 wt% glucose), exhibited the best photocatalytic performance for hydrogen production from water under visible light irradiation, which is about 4.55 times of that of the bulk g-C3N4 (BCN). The improvement of photocatalytic activity was mainly attributed to the construction of built-in electric field at the interface of CDs and g-C3N4, which could improve the separation of photogenerated electron-hole pair. Moreover, the tight connection of CDs with g-C3N4 would serve as a well electron transport channel, which could promote the photocatalytic H2 evolution ability.  相似文献   

19.
Mesoporous g-C3N4/Zn–Ti layered double hydroxide (LDH)-laminated van der Waals heterojunction nanosheets were prepared by a facile one-step in situ hydrothermal method. Due to the strong electrostatic interactions between the positively charged Zn–Ti LDH and negatively charged g-C3N4 nanocrystal, a laminated van der Waals heterostructure was successfully formed between Zn–Ti LDH and g-C3N4. The mesoporous g-C3N4/Zn–Ti LDH-laminated van der Waals heterojunction, which had a narrow bandgap of 2.41 eV extended the photoresponse to the visible light region. The obtained heterojunctions showed excellent visible-light-driven photocatalytic performance for the complete removal of ceftriaxone sodium (up to ∼97%) and a high hydrogen production rate (∼161.87 μmol h−1 g−1). This was mainly attributed to the formation of the laminated van der Waals heterojunctions, which favoured charge separation and the absorption of visible light, and the mesoporous structure, which provided more surface active sites. This facile strategy for preparing mesoporous g-C3N4/Zn–Ti LDH-laminated van der Waals heterojunctions offers new insights for the fabrication of high-performance van der Waals heterojunction photocatalytic materials.  相似文献   

20.
In this work, novel CuS/g-C3N4 composite photocatalysts were successfully prepared via a simple in-situ growth method. CuS nanoparticles, with an average diameter of ca.10 nm, were well dispersed on the surface of g-C3N4, revealing that g-C3N4 nanosheets were promising support for in-situ growth of nanosize materials. The CuS/g-C3N4 composites exhibited highly enhanced visible light photocatalytic H2 evolution from water-splitting compared to pure g-C3N4. The optimum photocatalytic activity of 2 wt% CuS/g-C3N4 composite photocatalytic H2 evolution was about 13.76 times higher than pure g-C3N4. The enhanced photocatalytic activity is attributed to the interfacial charge transfer (IFCT). In this system, electrons in the valence band (VB) of g-C3N4 can transfer directly to CuS clusters, causing the reduction of partial CuS to Cu2S, which can act as an electron sink and co-catalyst to promote the separation and transfer of photo-generated electrons. The accumulated photoinduced electrons in CuS/Cu2S clusters could effectively reduce H+ to produce H2. This work provides a possibility for constructing low-cost CuS as a substitute for noble metals in the photocatalytic production of H2 via a facile method based on g-C3N4.  相似文献   

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