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1.
A novel visible‐light‐driven g‐C3N4/MIL‐53(Al) composite photocatalyst was successfully prepared using a facile stirring method at room temperature. The g‐C3N4/MIL‐53(Al) composites were characterized and their effects on the photocatalytic activities for rhodamine B degradation were investigated. The g‐C3N4(20 wt%)/MIL‐53(Al) photocatalyst displayed optimal photocatalytic degradation efficiency, which was about five times higher than the photocatalytic activity of pure g‐C3N4. The improved photocatalytic performance of the g‐C3N4/MIL‐53(Al) photocatalyst was predominantly attributed to the efficient separation of electron–hole pairs and the low charge‐transfer resistance. g‐C3N4/MIL‐53(Al) also exhibited excellent stability and reusability. A proposed mechanism for the enhanced photocatalytic activity is also discussed based on the experimental results. Copyright © 2015 John Wiley & Sons, Ltd.  相似文献   

2.
From previous reports, graphitic carbon nitride (g‐C3N4) can be used as a photocatalyst, although the low efficiency of solar energy utilization, small specific surface area and high recombination rate of photogenerated electron–hole pairs limit its practical application. For the purpose of increasing photocatalytic activity, especially under irradiation of visible light, we successfully synthesized a new composite, namely porous g‐C3N4/Ag/Cu2O, through chemical adsorption of Ag‐doped Cu2O on porous g‐C3N4, which has not been investigated carefully worldwide. The composition, morphology and optical properties of the composite were investigated through methods including X‐ray diffraction, energy‐dispersive X‐ray, Fourier transform infrared, UV–visible and photoluminescence spectroscopies and transmission electron microscopy. Using rhodamine B as organic pollutant to be degraded under the irradiation of visible light, different mass ratios of Ag/Cu2O doped on porous g‐C3N4 led to enhanced photocatalytic performance of the composite compared to pure porous g‐C3N4. When the mass ratio of Ag/Cu2O is 15%, porous g‐C3N4/Ag/Cu2O exhibits a degradation rate 2.015 times higher than that of pure porous g‐C3N4. The reasons for this phenomenon may be attributed to the increased utilization efficiency of visible light, high‐speed separation of photogenerated electron–hole pairs, accelerated interfacial transfer process of electrons and increased surface area of the composite. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

3.
Herein, a novel broken case‐like carbon‐doped g‐C3N4 photocatalyst was obtained via a facile one‐pot pyrolysis and cost‐effective method using glyoxal‐modified melamine as a precursor. The obtained carbon/g‐C3N4 photocatalyst showed remarkable enhanced photocatalytic activity in the degradation of gaseous benzene compared with that of pristine g‐C3N4 under visible light. The pseudo‐first‐order rate constant for gaseous benzene degradation on carbon/g‐C3N4 was 0.186 hr?1, 5.81 times as large as that of pristine g‐C3N4. Furthermore, a possible photocatalytic mechanism for the improved photocatalytic performance over carbon/g‐C3N4 nanocomposites was proposed.  相似文献   

4.
As a metal‐free nitrogen reduction reaction (NRR) photocatalyst, g‐C3N4 is available from a scalable synthesis at low cost. Importantly, it can be readily functionalized to enhance photocatalytic activities. However, the use of g‐C3N4‐based photocatalysts for the NRR has been questioned because of the elusive mechanism and the involvement of N defects. This work reports the synthesis of a g‐C3N4 photocatalyst modified with cyano groups and intercalated K+ (mCNN), possessing extended visible‐light harvesting capacity and superior photocatalytic NRR activity (NH3 yield: 3.42 mmol g?1 h?1). Experimental and theoretical studies suggest that the ‐C≡N in mCNN can be regenerated through a pathway analogous to Mars van Krevelen process with the aid of the intercalated K+. The results confirm that the regeneration of the cyano group not only enhances photocatalytic activity and sustains the catalytic cycle, but also stabilizes the photocatalyst.  相似文献   

5.
Herein, for the first time, a direct Z‐scheme g‐C3N4/NiFe2O4 nanocomposite photocatalyst was prepared using facile one‐pot hydrothermal method and characterized using XRD, FT‐IR, DRS, PL, SEM, EDS, TEM, HRTEM, XPS, BET and VSM characterized techniques. The result reveals that the NiFe2O4 nanoparticles are loaded on the g‐C3N4 sheets successfully. The photocatalytic activities of the as‐prepared photocatalysts were evaluated for the degradation of methyl orange (MO) under visible light irradiation. It was shown that the photocatalytic activity of the g‐C3N4/NiFe2O4 nanocomposite is about 4.4 and 3 times higher than those of the pristine NiFe2O4 and g‐C3N4 respectively. The enhanced photocatalytic activity could be ascribed to the formation of g‐C3N4/NiFe2O4 direct Z‐scheme photocatalyst, which results in efficient space separation of photogenerated charge carriers. More importantly, the as‐prepared Z‐scheme photocatalyst can be recoverable easily from the solution by an external magnetic field and it shows almost the same activity for three consecutive cycles. Considering the simplicity of preparation method, this work will provide new insights into the design of high‐performance magnetic Z‐scheme photocatalysts for organic contaminate removal.  相似文献   

6.
Acid‐treated g‐C3N4‐Cu2O was prepared by hydrothermal reduction followed by high temperature calcination and acid exfoliation. The structures and properties of as‐synthesized samples were characterized using a range of techniques, such as X‐ray photoelectron spectroscopy, scanning electron microscopy, Photoluminescence Spectroscopy and the Brunauer–Emmett–Teller (BET) theory. The photocatalytic activity was evaluated by measuring the photodegradation of methyl orange under visible‐light irradiation. Based on the results of TEM, XPS, EPR and other techniques, it was verified that a heterojunction was formed. The acid treatment process can increase the specific surface area to form abundant heterojunction interfaces as channels for photo‐generated carrier separation, thereby enhancing its light utilization and quantum efficiency. Results indicate that acid‐treated g‐C3N4‐Cu2O possesses a large specific surface area, which provides plentiful activated sites for heterojunctions to form; in addition, it showed a high visible light effect and the minimum charge‐transfer resistance. Furthermore, the g‐C3N4‐Cu2O material exhibits high levels of effectiveness and stability. Electron paramagnetic resonance and a series of radical trapping experiments demonstrate that the holes and ?O2? could be the main active species in methyl orange photodegradation. This work could provide new insights into the fabrication of composite materials as high‐performance photocatalysts, and facilitate their application in addressing environmental protection issues.  相似文献   

7.
Introducing plasmonic metals into semiconductor materials has been proven to be an attractive strategy for enhancing photocatalytic activity in the visible region. In this work, a novel and efficient Ag/Ag2WO4/g‐C3N4 (AACN) ternary plasmonic photocatalyst was successfully synthesized using a facile one‐step in situ hydrothermal method. The composition, structure, morphology and optical absorption properties of AACN were investigated using X‐ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, and UV–visible diffuse reflectance spectroscopy, respectively. Photocatalytic performance of AACN was evaluated via rhodamine B and tetracycline degradation. The results indicated that AACN had excellent photocatalytic performance for rhodamine B degradation with a rate constant of 0.0125 min?1, which was higher than those of Ag2WO4 and Ag/Ag2WO4. Characterization and photocatalytic tests showed that the strong coupling effect between the Ag/Ag2WO4 nanoparticles and the exfoliated ultrathin g‐C3N4 nanosheets was superior for visible‐light responsivity and reduced the recombination rate of photogenerated electrons and holes. A proposed mechanism is also discussed according to the band energy structure and the experimental results.  相似文献   

8.
《化学:亚洲杂志》2017,12(3):361-365
In this work, graphitic C3N4 decorated with a CoP co‐catalyst (g‐C3N4/CoP) is reported for photocatalytic H2 evolution reaction based on two‐step hydrothermal and phosphidation method. The structure of g‐C3N4/CoP is well confirmed by XRD, FTIR, TEM, XPS, and UV/Vis diffuse reflection spectra techniques. When the weight percentage of CoP loading is 3.4 wt % (g‐C3N4/CoP‐3.4 %), the highest H2 evolution amount of 8.4×102 μmol g−1 is obtained, which is 1.1×103 times than that over pure g‐C3N4. This value also is comparable with that of g‐C3N4 loaded by the same amount of Pt. In cycling experiments, g‐C3N4/CoP‐3.4 % shows a stable photocatalytic activity. In addition, g‐C3N4/CoP‐3.4 % is an efficient photocatalyst for H2 evolution under irradiation with natural solar light. Based on comparative photoluminescence emission spectra, photoelectrochemical I –t curves, EIS Nyquist plots, and polarization curves between g‐C3N4/CoP‐3.4 % and pure g‐C3N4, it is concluded that the presence of the CoP co‐catalyst accelerates the separation and transfer of photogenerated electrons of g‐C3N4, thus resulting in improved photocatalytic activity in the H2 evolution reaction.  相似文献   

9.
Exploiting advanced photocatalysts under visible light is of primary significance for the development of environmentally relevant photocatalytic decontamination processes. In this study, the ionic liquid (IL), 1‐butyl‐3‐methylimidazolium tetrafluoroborate, was employed for the first time as both a structure‐directing agent and a dopant for the synthesis of novel fluorinated B/C‐codoped anatase TiO2 nanocrystals (TIL) through hydrothermal hydrolysis of tetrabutyl titanate. These TIL nanocrystals feature uniform crystallite and pore sizes and are stable with respect to phase transitions, crystal ripening, and pore collapse upon calcination treatment. More significantly, these nanocrystals possess abundant localized states and strong visible‐light absorption in a wide range of wavelengths. Because of synergic interactions between titania and codopants, the calcined TIL samples exhibited high visible‐light photocatalytic activity in the presence of oxidizing Rhodamine B (RhB). In particular, 300 °C‐calcined TIL was most photocatalytically active; its activity was much higher than that of TiO1.98N0.02 and reference samples (TW) obtained under identical conditions in the absence of ionic liquid. Furthermore, the possible photocatalytic oxidation mechanism and the active species involved in the RhB degradation photocatalyzed by the TIL samples were primarily investigated experimentally by using different scavengers. It was found that both holes and electrons, as well as their derived active species, such as .OH, contributed to the RhB degradation occurring on the fluorinated B/C‐codoped TiO2 photocatalyst, in terms of both the photocatalytic reaction dynamics and the reaction pathway. The synthesis of the aforementioned novel photocatalyst and the identification of specific active species involved in the photodegradation of dyes could shed new light on the design and synthesis of semiconductor materials with enhanced photocatalytic activity towards organic pollutants.  相似文献   

10.
Halide perovskite quantum dots (QDs) have great potential in photocatalytic applications if their low charge transportation efficiency and chemical instability can be overcome. To circumvent these obstacles, we anchored CsPbBr3 QDs (CPB) on NHx‐rich porous g‐C3N4 nanosheets (PCN) to construct the composite photocatalysts via N?Br chemical bonding. The 20 CPB‐PCN (20 wt % of QDs) photocatalyst exhibits good stability and an outstanding yield of 149 μmol h?1 g?1 in acetonitrile/water for photocatalytic reduction of CO2 to CO under visible light irradiation, which is around 15 times higher than that of CsPbBr3 QDs. This study opens up new possibilities of using halide perovskite QDs for photocatalytic application.  相似文献   

11.
In this study, the photocatalytic activity of graphitic carbon nitride (g‐C3N4) synthesized via different precursors (urea, thiourea, and dicyandiamide) is investigated in the degradation process of tetracycline. Owing to the efficient charge separation and transfer, prolonged radiative lifetime of charge, large surface area, and nanosheet morphology, the urea‐derived g‐C3N4 exhibits superior photocatalytic activity for tetracycline degradation under visible‐light irradiation. This performance can compare with that of most reported g‐C3N4‐based composite photocatalysts. Through the time‐circle degradation experiment, the urea‐derived g‐C3N4 is found to have an excellent photocatalytic stability. The presence of NO3?, CH3COO?, Cl? and SO42? ions with the concentration of 10 mm inhibits the photocatalytic activity of urea‐derived g‐C3N4, where this inhibitory effect is more obvious for Cl? and SO42? ions. For the coexisting Cu2+, Ca2+, and Zn2+ ions, the Cu2+ ion exhibits a significantly higher inhibitory effect than Ca2+ and Zn2+ ions for tetracycline degradation. However, both the inhibitory and facilitating effects are observed in the presence of Fe3+ ion with different concentration. The h+, .OH and .O2? radicals are confirmed as major oxidation species and a possible photocatalytic mechanism is proposed in a urea‐derived g‐C3N4 reaction system. This study is of important significance to promote the large‐scale application of g‐C3N4 photocatalysts in antibiotic wastewater purification.  相似文献   

12.
As a photocatalyst, mesoporous carbon nitride (mpg‐C3N4) shows higher photocatalytic activities in organic synthesis. Herein we report an mpg‐C3N4‐catalyzed oxidation of α‐hydroxy ketones to synthesize 1,2‐diketones using visible light. This transformation represents a green and highly efficient synthetic route to synthesize 1,2‐diketones for which catalytic approaches are scarce.  相似文献   

13.
Photodeposition has been widely used as a mild and efficient synthetic method to deposit co‐catalysts. It is also worth studying how to synthesize non‐noble metal photocatalysts with uniform dispersion. Different synthetic conditions in photodeposition have a certain influence on particle size distribution and photocatalytic activity. Therefore, we designed experiments to prepare the inexpensive composite photocatalyst Ni(OH)2/g‐C3N4 by photodeposition. The Ni(OH)2 co‐catalysts disperse uniformly with particle sizes of about 10 nm. The photocatalytic hydrogen production rate of Ni(OH)2/g‐C3N4 reached about 19 mmol g?1 h?1, with the Ni(OH)2 deposition amount about 1.57 %. During 16 h stability testing, the rate of hydrogen production did not decrease significantly. The composite catalyst also revealed a good hydrogen production performance under sunlight. The Ni(OH)2 co‐catalyst enhanced the separation ability of photogenerated carriers, which was proved by surface photovoltage and fluorescence analysis.  相似文献   

14.
Knowledge of the photocatalytic H2 evolution mechanism is of great importance for designing active catalysts toward a sustainable energy supply. An atomic‐level insight, design, and fabrication of single‐site Co1‐N4 composite as a prototypical photocatalyst for efficient H2 production is reported. Correlated atomic characterizations verify that atomically dispersed Co atoms are successfully grafted by covalently forming a Co1‐N4 structure on g‐C3N4 nanosheets by atomic layer deposition. Different from the conventional homolytic or heterolytic pathway, theoretical investigations reveal that the coordinated donor nitrogen increases the electron density and lowers the formation barrier of key Co hydride intermediate, thereby accelerating H–H coupling to facilitate H2 generation. As a result, the composite photocatalyst exhibits a robust H2 production activity up to 10.8 μmol h−1, 11 times higher than that of pristine counterpart.  相似文献   

15.
Heterojunction design in a two-dimensional (2D) fashion has been deemed beneficial for improving the photocatalytic activity of g-C3N4 because of the promoted interfacial charge transfer, yet still facing challenges. Herein, we construct a novel 2D/2D Cu3P nanosheet/P-doped g-C3N4 (PCN) nanosheet heterojunction photocatalyst (PCN/Cu3P) through a simple in-situ phosphorization treatment of 2D/2D CuS/g-C3N4 composite for photocatalytic H2 evolution. We demonstrate that the 2D lamellar structure of both CuS and g-C3N4 could be well reserved in the phosphorization process, while CuS and g-C3N4 in-situ transformed into Cu3P and PCN, respectively, leading to the formation of PCN/Cu3P tight 2D/2D heterojunction. Owing to the large contact area provided by intimate face-to-face 2D/2D structure, the PCN/Cu3P photocatalyst exhibits significantly enhanced charge separation efficiency, thus achieving a boosted visible-light-driven photocatalytic behavior. The highest rate for H2 evolution reaches 5.12 μmol·h–1, nearly 24 times and 368 times higher than that of pristine PCN and g-C3N4, respectively. This work represents an excellent example in elaborately constructing g-C3N4-based 2D/2D heterostructure and could be extended to other photocatalyst/co-catalyst system.   相似文献   

16.
用酸催化溶胶-凝胶法制备了Fe3+掺杂TiO2/凹凸棒(Fe3+-TiO2/ATP)复合光催化剂,对其结构、微观形貌、光吸收性能和可见光下的光催化性能进行了表征。XRD和TEM测试结果表明,Fe3+-TiO2/ATP具有较好的热稳定性,经450 ℃热处理后的ATP晶体结构基本保持不变,锐钛矿TiO2均匀的分布在ATP表面,TiO2颗粒之间无团聚,且平均粒径小于纯TiO2。UV-Vis-DRS测试结果表明,Fe3+的掺杂可明显增强复合光催化剂对可见光的吸收,光响应范围拓展到了整个紫外-可见光区。在可见光下,Fe3+-TiO2/ATP复合光催化剂对亚甲基蓝具有很好的催化降解活性。Fe3+-TiO2/ATP的反应速率常数分别为TiO2/ATP、P25和纯TiO2的1.37、4.83和6.51倍。复合光催化剂的沉降性能优于纯TiO2和P25,易于分离。  相似文献   

17.
The photocatalytic activity of graphite‐like carbon nitride (g‐C3N4) could be enhanced by heterojunction strategies through increasing the charge‐separation efficiency. As a surface‐based process, the heterogeneous photocatalytic process would become more efficient if a larger contact region existed in the heterojunction interface. In this work, ultrathin g‐C3N4 nanosheets (g‐C3N4‐NS) with much larger specific surface areas are employed instead of bulk g‐C3N4 (g‐C3N4‐B) to prepare AgIO3/g‐C3N4‐NS nanocomposite photocatalysts. By taking advantage of this feature, the as‐prepared composites exhibit remarkable performances for photocatalytic wastewater treatment under visible‐light irradiation. Notably, the optimum photocatalytic activity of AgIO3/g‐C3N4‐NS composites is almost 80.59 and 55.09 times higher than that of pure g‐C3N4‐B towards the degradation of rhodamine B and methyl orange pollutants, respectively. Finally, the stability and possible photocatalytic mechanism of the AgIO3/g‐C3N4‐NS system are also investigated.  相似文献   

18.
The structures of five compounds consisting of (prop‐2‐en‐1‐yl)bis[(pyridin‐2‐yl)methylidene]amine complexed with copper in both the CuI and CuII oxidation states are presented, namely chlorido{(prop‐2‐en‐1‐yl)bis[(pyridin‐2‐yl)methylidene]amine‐κ3N,N′,N′′}copper(I) 0.18‐hydrate, [CuCl(C15H17N3)]·0.18H2O, (1), catena‐poly[[copper(I)‐μ2‐(prop‐2‐en‐1‐yl)bis[(pyridin‐2‐yl)methylidene]amine‐κ5N,N′,N′′:C2,C3] perchlorate acetonitrile monosolvate], {[Cu(C15H17N3)]ClO4·CH3CN}n, (2), dichlorido{(prop‐2‐en‐1‐yl)bis[(pyridin‐2‐yl)methylidene]amine‐κ3N,N′,N′′}copper(II) dichloromethane monosolvate, [CuCl2(C15H17N3)]·CH2Cl2, (3), chlorido{(prop‐2‐en‐1‐yl)bis[(pyridin‐2‐yl)methylidene]amine‐κ3N,N′,N′′}copper(II) perchlorate, [CuCl(C15H17N3)]ClO4, (4), and di‐μ‐chlorido‐bis({(prop‐2‐en‐1‐yl)bis[(pyridin‐2‐yl)methylidene]amine‐κ3N,N′,N′′}copper(II)) bis(tetraphenylborate), [Cu2Cl2(C15H17N3)2][(C6H5)4B]2, (5). Systematic variation of the anion from a coordinating chloride to a noncoordinating perchlorate for two CuI complexes results in either a discrete molecular species, as in (1), or a one‐dimensional chain structure, as in (2). In complex (1), there are two crystallographically independent molecules in the asymmetric unit. Complex (2) consists of the CuI atom coordinated by the amine and pyridyl N atoms of one ligand and by the vinyl moiety of another unit related by the crystallographic screw axis, yielding a one‐dimensional chain parallel to the crystallographic b axis. Three complexes with CuII show that varying the anion composition from two chlorides, to a chloride and a perchlorate to a chloride and a tetraphenylborate results in discrete molecular species, as in (3) and (4), or a bridged bis‐μ‐chlorido complex, as in (5). Complex (3) shows two strongly bound Cl atoms, while complex (4) has one strongly bound Cl atom and a weaker coordination by one perchlorate O atom. The large noncoordinating tetraphenylborate anion in complex (5) results in the core‐bridged Cu2Cl2 moiety.  相似文献   

19.
A novel and facile method was developed to prepare a visible‐light driven TiO2/Ag‐AgCl@polypyrrole (PPy) photocatalyst with Ag‐AgCl nanoparticles supported on TiO2 nanofibers and covered by a thin PPy shell. During the synthesis, the PPy shell and Ag‐AgCl nanoparticles were prepared simultaneously onto TiO2 nanofibers, which simplified the preparation procedure. In addition, because Ag‐AgCl aggregates were fabricated via partly etching the Ag nanoparticles, their size was well controlled at the nanoscale, which was beneficial for improvement of the contact surface area. Compared with reference photocatalysts, the TiO2/Ag‐AgCl@PPy composite exhibited an enhanced photodegradation activity towards rhodamine B under visible‐light irradiation. The superior photocatalytic property originated from synergistic effects between TiO2 nanofibers, Ag‐AgCl nanoparticles and the PPy shell. Furthermore, the TiO2/Ag‐AgCl@PPy composite could be easily separated and recycled without obvious reduction in activity.  相似文献   

20.
A heterogeneous photocatalyst system that consists of a ruthenium complex and carbon nitride (C3N4), which act as the catalytic and light‐harvesting units, respectively, was developed for the reduction of CO2 into formic acid. Promoting the injection of electrons from C3N4 into the ruthenium unit as well as strengthening the electronic interactions between the two units enhanced its activity. The use of a suitable solvent further improved the performance, resulting in a turnover number of greater than 1000 and an apparent quantum yield of 5.7 % at 400 nm. These are the best values that have been reported for heterogeneous photocatalysts for CO2 reduction under visible‐light irradiation to date.  相似文献   

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