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.
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   

2.
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   

3.
The design of p-n heterojunction photocatalysts to overcome the drawbacks of low photocatalytic activity that results from the recombination of charge carriers and narrow photo-response range is promising technique for future energy. Here, we demonstrate the facile hydrothermal synthesis for the preparation of Bi2O3/MoS2 p-n heterojunction photocatalysts with tunable loading amount of Bi2O3 (0–15 wt%). The structure, surface morphology, composition and optical properties of heterostructures were studied using X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), UV–visible absorption spectroscopy, Brunauer-Emmett-Teller (BET) surface area, photoluminescence (PL), electrochemical impedance spectroscopy (EIS). Compare to pure Bi2O3 and MoS2, the Bi2O3/MoS2 heterostructures displayed significantly superior performance for photocatalytic hydrogen (H2) production using visible photo-irradiation. The maximum performance for hydrogen evolution was achieved over Bi2O3/MoS2 photocatalyst (10 μmol h−1g−1) with Bi2O3 content of 11 wt%, which was approximately ten times higher than pure Bi2O3 (1.1 μmol h−1g−1) and MoS2 (1.2 μmol h−1g−1) photocatalyst. The superior performance was attributed to the robust light harvesting ability, enhanced charge carrier separation via gradual charge transferred pathway. Moreover, the increased efficiency of Bi2O3/MoS2 heterostructure photocatalyst is discussed through proposed mechanism based on observed performance, band gap and band position calculations, PL and EIS data.  相似文献   

4.
The present study has successfully fabricated a Cu2-xSe/rGO heterojunction for the first time using an in situ hot-injection method and employed it to produce photocatalytic hydrogen. The optimal Cu2-xSe/3%rGO can achieve an efficient photocatalytic H2 production at the rate 3123.48 μmol g−1 h−1, nearly 3.46 times higher than that of the pure Cu2-xSe. The enhanced activity can be attributed to facilitated light absorption, up-regulated charge density, lower interfacial transfer resistance as well as a longer electron decay lifetime. In the meantime, the expanded specific surface area can create more active reaction sites, leading to the enhancement of photocatalytic peropeties. Besides, the mechanism of the Cu2-xSe/rGO heterojunction's hydrogen production is proposed.  相似文献   

5.
An oxygen-vacancy rich, bismuth oxide (Bi2O3) based MoS2/Bi2O3 Z-scheme heterojunction catalyst (2-BO-MS) was prepared in an autoclave hydrothermal method using ethanol and water. The performance of MoS2/Bi2O3 catalyst was examined for photocatalytic hydrogen evolution, photoelectrochemical activity, and crystal violet (CV) dye degradation by comparing with pristine Bi2O3 and MoS2. The hydrogen evolution performances of 2-BO-MS catalyst exhibited 3075.21 μmol g−1 h−1, which is 7.18 times higher than that of MoS2 (428.14 μmol g−1 h−1). The XPS, XRD and HRTEM analyses covered that the superior photocatalytic performance of 2-BO-MS catalyst might have stemmed out due to the existence of oxygen vacancies, enhanced strong interfacial interaction between MoS2 and Bi2O3 and specific surface area. The in-depth investigation has been performed for MoS2/Bi2O3 Z-scheme heterojunction using several characterization techniques. Moreover, the photocatalytic mechanism for hydrogen evolution and photodegradation were proposed based on trapping experiment results. This results acquired using MoS2/Bi2O3 Z-scheme heterojunction would be stepping stone for developing heterojunction catalyst towards attaining outstanding photocatalytic activity.  相似文献   

6.
In this work, photocatalysts with a novel S-scheme heterojunction were fabricated by coupling MOF-derived TiO2 with porous g-C3N4 (MTO/PCN). The S-scheme heterojunction with matching band gap possesses different advantageous properties, which can not only inhibit photo-generated charge recombination, but also reserve outstanding redox ability. As expected, superior hydrogen evolution efficiency of 40-MTO/PCN was obtained in a TEOA-containing aqueous solution and pure water, which were 5252.9 and 974.6 μmol h−1 g−1, respectively. Meanwhile, the hybrid can also serve as a bifunctional catalyst for H2 generation (2137.3 μmol h−1 g−1) and organic contaminant removal (the RhB purification efficiency: 35.24%). This work furnishes a feasible method for devising bifunctional photocatalysts that can simultaneously produce hydrogen and purify wastewater to provide both energy-saving and environmental restoration functions.  相似文献   

7.
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   

8.
A novel and porous triptycene-based microporous polymer (TMP) was synthesized through a palladium acetate-catalyzed Suzuki reaction, and then Cd0.5Zn0.5S quantum dots (CZS QDs) were homogeneously decorated onto the TMP by a facile in situ precipitation approach to fabricate a 0D/3D heterojunction for the first time. Characterizations indicate TMP with large specific surface area (809 m2 g−1) not only stabilizes CZS QDs but also provides abundant photocatalytic active sites, which can facilitate the activation and adsorption of H2O molecules. The CZS QDs@TMP heterojunction possesses remarkably improved photocatalytic hydrogen evolution activity and outstanding photostability. The optimized CZS QDs@TMP-1 heterojunction exhibits highest hydrogen-producing rate of 81.33 mmol h−1 g−1, about 16.1 times higher than that of pristine CZS. The high photocatalytic activity of CZS QDs@TMP is due to several positive factors, such as high surface area, construction of n-n type heterostructures, tiny size effect of CZS QDs and close contact between 0D CZS QDs and 3D TMP, which will synergistically promote the visible-light response, boost the interfacial charge transfer and reduce the photocorrosion of CZS.  相似文献   

9.
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   

10.
In this paper, a novel 2D bubble-like g-C3N4 (B–CN) with a highly porous and crosslinked structure is successfully synthesized via a cost-effective bottom-up process. The as-prepared B–CN photocatalyst delivers a considerably expanded specific surface area and increased active sites. Moreover, the 2D bubble-like structure can afford shortened diffusion paths for both photogenerated charge carriers and reactants. As a result, the photocatalytic H2 evolution rate of B–CN reached 268.9 μmol g?1 h?1, over 5 times more than that of bulk C3N4. The Ni ions were further deposited on B–CN as a cocatalyst to enhance the photocatalytic activity. Benefit from the synergy of 2D bubble-like structure and Ni species cocatalyst, recombination of photoinduced charges was greatly inhibited and the hydrogen evolution reaction (HER) was significantly accelerated. The resulted catalyst achieved a dramatically high H2 evolution rate of 1291 μmol g?1 h?1. This work provides an alternative way to synthesize novel porous carbon nitride together with non-noble metal cocatalysts toward enhanced photocatalytic activity for H2 production.  相似文献   

11.
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   

12.
Graphitic carbon nitride tetragonal hollow prism (GCN-THP) with nitrogen vacancies was prepared by a simple two-step calcination method. Based on the characterizations of the as-prepared GCN-THP and the intermediate precursor, a possible mechanism was proposed for the formation of GCN-THP. The as-prepared GCN-THP exhibits superior activity and excellent stability during photocatalytic hydrogen evolution under visible light irradiation. The photocatalytic hydrogen evolution rate of GCN-THP was measured to be 1990 μmol g−1 h−1, which is 6.2 times as that of GCN. The enhanced photocatalytic activity could be attributed to unique 1D tetragonal hollow prism morphology and the presence of nitrogen vacancies in the as-prepared GCN-THP, which could increase the surface area, expand the visible light absorption, and promote the charge separation during photocatalytic hydrogen evolution. Our work could provide a new route to synthesize highly efficient photocatalysts with 1D hollow structures.  相似文献   

13.
The construction of p-n type heterojunction is an effective way to enhance the efficiency of photocatalytic hydrogen evolution. In this work, Co3O4/CeO2 p-n heterojunction was construct by a simple hydrothermal method. This heterojunction mainly uses the internal electric field formed and accelerate the separation of electrons and holes in the opposite direction. In addition, according to SEM and TEM characterization, it was found that the granular cobalt oxide nanoparticles prepared by in-situ hydrothermal method were firmly and uniformly dispersed in cerium oxide, which effectively increased the active sites of hydrogen evolution. And combined with the BET results, it shows that the growth of cobalt oxide effectively increases the specific surface area and increases the active sites for hydrogen evolution. By exploring the hydrogen evolution capacity of different ratios of the complex, the test results showed that in all different ratios of the catalyst, CC-0.16 showed the best performance, and the hydrogen production efficiency reached 2298.52 μmol g−1h−1, which was 71 times that of nanobelt CeO2 and 2.72 times that of Co3O4. According to the characterization results, the photocatalytic water splitting mechanism of the p-n heterojunction was proposed, and the charge transfer mechanism in the process was discussed in depth.  相似文献   

14.
Overcoming the low charge transfer efficiency and poor photothermal stability of halide perovskite quantum dots (QDs) is the booster to achieve photocatalytic applications. In this paper, the Pt2+-doped CsPbBr3 QDs/two-dimensional accordion-like Ni-MOF (CPPB QDs/Ni-MOF) composite was firstly synthesized by fixing the CPPB QDs into the pores of Ni-MOF. Electron separation and transfer efficiency were analyzed by PL spectra and electrochemical data. The photocatalyst exhibited outstanding photocatalytic performance in hydrogen (H2) evolution. The optimal H2 evolution efficiency of the composite reached 153.6 μmol h?1, which was about 9 times than that of pure Ni-MOF and remained 134.8 μmol h?1 after the cycle test. The splendid efficiency could be benefited from the advantages of 2D layered structure of Ni-MOF and the high charge separation and transmission efficiency of CPPB QDs. Finally, the mechanism of electron migration and additional electron transfer channels between composite interfaces was further demonstrated by density functional theory (DFT) calculations. The present work opens up a novel perspective for photocatalytic applications of doped halide perovskite QDs/Ni-MOF nanocomposites.  相似文献   

15.
Constructing S-scheme heterojunction is regarded as an effective mode to motivate excellent photocatalytic performance for hydrogen generation. This paper prepares NiTiO3/CdIn2S4 S-scheme heterostructure photocatalyst by hydrothermal method successfully. In the experiments, 20 wt% NiTiO3/CdIn2S4 has the supreme photocatalytic activity with the H2 generation rate of 5168.6 μmol g−1 h−1 and the apparent quantum yield (AQY) of 5.14% at 420 nm, approximately 7.7 times of pure CdIn2S4. Through the phase characterization analyses, NiTiO3 and CdIn2S4 successfully compounded, with NiTiO3 nanoparticles wrapping around CdIn2S4 microspheres to form the irregular clumps. Further analyses of performance reveal the larger specific surface area, wider absorption region, faster charge transfer rate, outstanding photostability and recyclability for 20 wt% NiTiO3/CdIn2S4, all of which play the significant role in photocatalytic hydrogen evolution activity. Finally, a plausible S-scheme photocatalytic mechanism for NiTiO3/CdIn2S4 is proposed. This study provides a novel and effective S-scheme photocatalyst for hydrogen generation from water splitting.  相似文献   

16.
The main challenge of photocatalysis is how to improve the coefficient of utilization and conversion rate for solar energy. Herein, we report a composite photocatalyst related to a novel porphyrin metal organic frameworks (MOFs), in which cadmium sulfide nanoparticles (CdS NPs) are grown in situ on the surface of two-dimensional (2D) zinc porphyrin nanosheets (Zn-TCPP NSs) by hydrothermal method. Interestingly, Zn-TCPP NSs and CdS NPs form a Type II heterojunction structure, which reduces the photogenerated electron-hole recombination rate of CdS. Moreover, in the near-infrared region, the photo-excited electrons generated by Zn-TCPP NSs are transmitted to CdS NPs, so that cadmium sulfide can realize both visible light and near-infrared light for photocatalytic hydrogen production. The Zn-TCPP NSs not only has excellent light absorption capacity, but also has a unique frame design that effectively reduces the recombination rate of photoinduced electron hole pairs, thus improving the conversion rate of solar energy. As expected, the photocatalytic performance of the porphyrin MOFs modified materials is significantly enhanced compared to CdS NPs. The hydrogen production rate of the Pt@CdS NPs/Zn-TCPP NSs(C-Z-T) composite material in the visible light region is about 15.3 mmol g?1 h?1, which is 11 times for Pt@CdS NPs. Furthermore, the Pt@CdS NPs/Zn-TCPP NSs(C-Z-T) also has a considerable hydrogen production rate in the near-infrared region, such as 200 μmol g?1 h?1 at 600 nm, 90 μmol g?1 h?1 at 765 nm and 20 μmol g?1 h?1 at > 800 nm.  相似文献   

17.
Modifying the texture of carbon nitride to adjust its physicochemical performance is a fascinating method for achieving high photocatalytic activity. Herein, we synthesized 3D porous carbon nitride with ultra-thin nanosheets by using cyanuric acid-melamine supramolecular and ionic liquid as precursor and template, respectively. The ionic liquid adjusts the morphology of materials and induces the carbon residue into the porous channels owing to its incomplete degradation. The 3D porous framework makes carbon nitride reflect the enhanced surface area, exposes adequate reaction sites, and offers a pathway for charge transport. And carbon residue and ultra-thin nanosheets further promote the photogenerated carriers transport and reduce the recombination rate of charge carriers. Consequently, 3D porous carbon nitride with ultra-thin nanosheets exhibit outstanding and stable hydrogen evolution under visible light irradiation. Significantly, as-fabricated sample CN-100 reflects an improved H2 generation rate, up to 17,028 μmol h?1 g?1, which is 12 times higher than that of CN (1412 μmol h?1 g?1). The present work offers a unique synthesis strategy to develop the novel photocatalyst with efficient photocatalytic performance.  相似文献   

18.
Carbon quantum dots (CQDs) have attracted growing interest due to their superior luminescent properties, which make them excellent photosensitizers for TiO2. This study presents the green-synthesis of CQDs from edible mushroom Agaricus bisporus through microwave irradiation. In the study as-synthesized CQDs were used as a sensitizer for TiO2 in photocatalytic hydrogen evolution in aqueous triethanolamine (sacrificial reagent) under visible-light irradiation. Photocatalytic hydrogen production activity of CQD-sensitized TiO2 was found to be 472 μmol g−1 h−1 (without loading any noble metal co-catalyst) and 1458 μmol g−1 h−1 (with loading Pt co-catalyst). The study revealed that the CQDs from mushroom A. bisporus can be used as an efficient sensitizer for TiO2 in photocatalytic hydrogen production.  相似文献   

19.
Novel heterogeneous structure of BiFeO3–CdWO4 with different molar ratios was applied for the photocatalytic hydrogen evolution in a self-designed externally UV/visible irradiated photoreactor in the presence of potassium iodide. The photocatalysts were synthesized by simple hydrothermal method and characterized by XRD, FE-SEM-mapping, TEM, UV–Vis DRS, PL, EIS, transient photocurrent and Mott-schottky techniques to identify the structural, optical and photoelectrochemical properties. The slope of Mott-schottky plots confirmed the p-type and n-type conductivity of the synthesized BiFeO3 and CdWO4, respectively. The p-n heterojunctions exhibited more efficiently light absorption, charge separation and electron mobility relative to the pure photocatalysts. We observed that coupling 40 mol% BiFeO3 with CdWO4 provided the best photocatalytic performance of hydrogen evolution, 268.90 μmol h−1.gcat−1 from distilled water and 379.43 μmol h−1.gcat−1 from 0.05 M KI aqueous solution. Iodine species increased H2 evolution efficiency because of taking part in the charge transfer processes, either by scavenging excited holes or by direct reduction of H+ to H under UV irradiation. Fermi level equilibrium in the p-n heterojunction suggests the best interparticle charge transfer mechanism explaining how photoinduced electrons with superior energy states and desirable lifetime can be supplied to reduce H+ to H.  相似文献   

20.
Tri-doped photocatalyst, SrTiO3:Ni/Ta/La, was prepared by spray pyrolysis from aqueous and polymeric precursor solutions. The third dopant, La3+, contributed to the BET surface area and porous morphology by preventing crystal growth, and increased the Ni2+/Ni3+ ratio by affecting the electron configuration in the lattice structure, which is closely related to the hydrogen evolution rate. The hydrogen evolution rate of the tri-doped photocatalyst, SrTiO3:Ni(0.2 mol%)/Ta(0.4 mol%)/La(0.3 mol%), was increased by about 60%–895.2 μmol g−1 h−1 from the value of 561.2 μmol g−1 h−1 for the co-doped photocatalyst, SrTiO3:Ni(0.2 mol%)/Ta(0.4 mol%), and was further enhanced to 2305.7 μmol g−1 h−1 when a polymeric precursor was used instead of an aqueous precursor in spray pyrolysis. The optimum additive content for polymeric precursor solution was 300 mol%.  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