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1.
Graphite-like C3N4 (g-C3N4) is ané cient visible-light-driven photocatalyst which is com-monly used in pollutant degradation. The photoreactivity of g-C3N4 depends on the prepa-ration conditions to a large extent. In this work, we linked the preparation conditions of g-C3N4 to its stability and photocatalytic activity through dye photodegradation experi-ments and sensitivity mathematical analyses. The sensitivity mathematical analyses show that the effect of calcination temperature is more significant than calcination time on the photoreactivity of g-C3N4. The photocatalytic activity of optimized g-C3N4 in rhodamine B (RhB) degradation under visible light was 100 times higher than that of non-optimized one. The enhanced performance can be attributed to the increased specific surface area of g-C3N4 and the increased migration velocity of photogenerated electron-hole pairs on the surface. This work deepens the understanding of the relation between preparation conditions and the charateristics of g-C3N4, and provides an extremely simple method for significantly improving the photoreactivity of g-C3N4.  相似文献   

2.
采用g-C_3N_4纳米片与聚丙烯腈进行静电复合纺丝,再经预氧化和碳化制得g-C_3N_4/C纳米纤维。利用傅立叶变换红外光谱仪(FTIR)、X射线衍射仪(XRD)、拉曼光谱(Raman)和扫描电子显微镜(SEM)对样品结构和形貌进行表征,通过紫外-可见漫反射光谱(UV-Vis DRS)分析可见光响应性。研究表明,复合纳米纤维对罗丹明B表现出较好的可见光降解活性,源于无定形相/石墨相混合结构的碳基体能够降低g-C_3N_4的光生电子-空穴对复合的几率。复合纳米纤维膜在光催化降解搅拌条件下始终能保持完整,经过多次回收和光催化实验,对罗丹明B的光降解率依然较高,表现出较优异的循环利用稳定性。  相似文献   

3.
采用g-C3N4纳米片与聚丙烯腈进行静电复合纺丝,再经预氧化和碳化制得g-C3N4/C纳米纤维。利用傅立叶变换红外光谱仪(FTIR)、X射线衍射仪(XRD)、拉曼光谱(Raman)和扫描电子显微镜(SEM)对样品结构和形貌进行表征,通过紫外-可见漫反射光谱(UV-Vis DRS)分析可见光响应性。研究表明,复合纳米纤维对罗丹明B表现出较好的可见光降解活性,源于无定形相/石墨相混合结构的碳基体能够降低g-C3N4的光生电子-空穴对复合的几率。复合纳米纤维膜在光催化降解搅拌条件下始终能保持完整,经过多次回收和光催化实验,对罗丹明B的光降解率依然较高,表现出较优异的循环利用稳定性。  相似文献   

4.
Using SBA-15 as a template, high surface area porous graphitic carbon nitrides (g-C3N4) were successfully synthesized by pretreating melamine using hydrochloric acid, and fully characterized by Fourier-Transform infrared (FT-IR), X-ray diffraction (XRD), scanning electron micrographs (SEM), N2 adsorption-desorption, ultraviolet-visible (UV-Vis) spectroscopy, photoluminescence (PL) spectrum. The results of these analyses indicated that the g-C3N4 synthesized from HCl-pretreated melamine with SBA-15 as a template has enhanced specific surface area and increased the separation rate of the photogenerated electrons and holes compared with bulk g-C3N4, but didn’t change the structure of bulk g-C3N4. The photocatalytic activity of samples was evaluated by the degradation of rhodamine B (RhB) under xenon lamp. The results indicated that the activity was improved significantly with the increase of specific surface area. The rate constant for CN-3(HCl pretreatment melamine precursor and SBA-15 as a template) was 13 times as high as g-C3N4. Furthermore, the CN-3 catalyst exhibited outstanding structural and catalytic stability.  相似文献   

5.
Highly efficient photocatalyst of visible-light-driven Ag nanoparticles loaded on porous graphitic carbon nitride (g-C3N4) was prepared by the reduction of Ag ions on porous g-C3N4. The obtained Ag/porous g-C3N4 composite products were characterized by X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), UV-vis diffuse reflection spectra (DRS), thermal gravimetric analysis (TGA). The results demonstrated that a homogeneous distribution of Ag NPs of 10 nm was attached onto the surface of the porous g-C3N4. The prepared Ag/porous g-C3N4 samples were applied for catalyzing the degradation of phenol in water under visible light irradiation. Porous g-C3N4 demonstrated an excellent support for the formation and dispersion of small uniform Ag NPs. When the weight percentage of Ag reaches 5%, the nanohybrid exhibits superior photocatalytic activities compared to bulk g-C3N4, porous g-C3N4, and 2% Ag/porous g-C3N4 hybrids. The enhanced photocatalytic performance is due to the synergic effect between Ag and porous g-C3N4, which suppressed the recombination of photogenerated electron-hole pairs.  相似文献   

6.
Direct Z-scheme g-C3N4/TiO2 nanorod composites were prepared for enhancing photocatalytic activity for pollutant removal. The characterization revealed that the g-C3N4/TiO2 nanorod composite formed a close interface contact between g-C3N4 and TiO2 nanorods, which was of benefit for the charge transfer and resulted in its high photocatalytic activity. The g-C3N4/TiO2 nanorod composites exhibited higher photocatalytic activity for degradation of Rhodamine B (RHB) than bare g-C3N4 and TiO2 nanorods. The high photocatalytic activity of g-C3N4/TiO2 nanorod composites is attributed to the formation of the direct Z-scheme system, in which the electrons from the conduction band (CB) of TiO2 combine with the holes from the valence band (VB) of C3N4 while the electrons from the CB of C3N4 and holes from the VB of TiO2 with stronger redox ability are used to reduce and oxidize pollutants. Based on the radical-trapping experiments, the main reactive species for RHB degradation are O2 and · OH, which are produced by photoinduced electrons and holes with high redox ability. This work provides insights into the photocatalytic mechanism of composite materials for the photocatalytic removal of organic pollutants.  相似文献   

7.
利用原位沉积法将BiOBr纳米片生长到g-C3N4表面,制得g-C3N4-BiOBr p-n型异质结复合光催化剂。采用X射线衍射(XRD)、红外光谱(FTIR)、场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)、紫外可见漫反射(UV-Vis-DRS)和荧光光谱(PL)等测试对光催化剂结构和性能进行表征。通过可见光辐照降解甲基橙水溶液检测评估复合光催化剂光催化活性。研究结果表明:复合光催化剂由BiOBr和g-C3N4两相组成,BiOBr纳米片在片状g-C3N4表面快速形核生长形成面-面复合结构。相比于纯相g-C3N4和BiOBr,g-C3N4-BiOBr复合材料具有更强可见光吸收能力,吸收带边红移。在可见光辐照100 min后,性能最佳的2:8 g-C3N4-BiOBr复合光催化剂光催化活性分别是纯相g-C3N4和BiOBr的1.8和1.2倍,经过4次循环实验后,其降解率仍达84%,说明复合结构光催化剂催化性能和稳定性增强。复合光催化剂的荧光强度显著降低,说明光生载流子复合得到了有效抑制。复合光催化剂催化性能的提高归因于p-n型异质结促进电荷有效分离、抑制电子-空穴复合和吸收光波长范围的扩展,相比单一成分材料具有更好的催化活性和稳定性。自由基捕获实验证明,可见光降解甲基橙光催化过程中的主要活性成分为空穴,并据此提出了可能的光催化机理。  相似文献   

8.
利用原位沉积法将Bi OBr纳米片生长到g-C_3N_4表面,制得g-C_3N_4-Bi OBr p-n型异质结复合光催化剂。采用X射线衍射(XRD)、红外光谱(FTIR)、场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)、紫外可见漫反射(UV-Vis-DRS)和荧光光谱(PL)等测试对光催化剂结构和性能进行表征。通过可见光辐照降解甲基橙水溶液检测评估复合光催化剂光催化活性。研究结果表明:复合光催化剂由Bi OBr和g-C_3N_4两相组成,Bi OBr纳米片在片状g-C_3N_4表面快速形核生长形成面-面复合结构。相比于纯相g-C_3N_4和Bi OBr,g-C_3N_4-Bi OBr复合材料具有更强可见光吸收能力,吸收带边红移。在可见光辐照100 min后,性能最佳的2:8 gC_3N_4-Bi OBr复合光催化剂光催化活性分别是纯相g-C_3N_4和Bi OBr的1.8和1.2倍,经过4次循环实验后,其降解率仍达84%,说明复合结构光催化剂催化性能和稳定性增强。复合光催化剂的荧光强度显著降低,说明光生载流子复合得到了有效抑制。复合光催化剂催化性能的提高归因于p-n型异质结促进电荷有效分离、抑制电子-空穴复合和吸收光波长范围的扩展,相比单一成分材料具有更好的催化活性和稳定性。自由基捕获实验证明,可见光降解甲基橙光催化过程中的主要活性成分为空穴,并据此提出了可能的光催化机理。  相似文献   

9.
The graphitic carbon nitride (g-C3N4) materials with many intriguing properties have attracted much attention in photocatalysis. The photocatalytic activity of g-C3N4 is hindered by serious aggregation and limited exposed active sites. Herein is shown that nanosized g-C3N4 can be simply obtained by a superfast high-pressure homogenization approach. The high-pressure homogenization treatment can provide strong force to cut and/or to exfoliate the bulk g-C3N4 into nanosized g-C3N4 with good dispersion. Moreover, choosing different solvents during treatment can cause a different surface structure of as-prepared nanosized g-C3N4. In addition, the narrow bandgap properties, the high photogenerated charge carrier separation, and the transport abilities are achieved in as-prepared nanosized g-C3N4 because of the retaining conjugated C3N4 system. Specifically, the photocatalytic activities of as-prepared nanosized g-C3N4 have been significantly enhanced in terms of degradation of organic dye Rhodamine B (RhB) under visible light irradiation (10 times higher than that of bulk g-C3N4). These findings can provide a promising and simple approach to the exfoliation, nanonization, and surface functionalization of 2D layered materials.  相似文献   

10.
以三聚氰胺和六水合氯化钴为原料,一锅法制备Co_3O_4负载的多孔石墨相氮化碳(Co_3O_4/g-C_3N_4)复合光催化材料。采用X射线衍射(XRD)、傅里叶变换红外(FT-IR)光谱、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、紫外-可见漫反射光谱(UV-Vis DRS)、光致发光光谱(PL)等手段对其结构和光学特性进行表征。以盐酸四环素(TC)为目标污染物,评价了不同负载量Co_3O_4/g-C_3N_4复合光催化剂的可见光催化性能。结果表明,所制备的Co_3O_4/g-C_3N_4复合光催化剂为多孔结构,其比表面积较大,并在可见光区域具有显著的吸收。利用原位生成的Co_3O_4纳米粒子在氮化碳表面形成异质结构,可有效转移光生载流子,降低光生电子-空穴的再结合率,从而提高光催化活性。并且存在最佳Co_3O_4复合量,当六水合氯化钴加入量为三聚氰胺的8%(w/w)时,所制备的复合光催化剂CoCN-8具有最佳的光催化性能。在可见光的照射下,60 min内可降解85%的TC,而同样条件下,纯g-C_3N_4仅降解23%的TC。  相似文献   

11.
Graphitic carbon nitride (g-C3N4) photocatalysts were synthesized via a one-step pyrolysis process using melamine, dicyandiamide, thiourea, and urea as precursors. The obtained g-C3N4 materials exhibited a significantly different performance for the photocatalytic reduction of Cr(VI) under white light irradiation, which is attributed to the altered structure and occupancies surface groups. The urea-derived g-C3N4 with nanosheet morphology, large specific surface area, and high occupancies of surface amine groups exhibited superior photocatalytic activity. The nanosheet morphology and large surface area facilitated the separation and transmission of charge, while the high occupancies of surface amine groups promoted the formation of hydrogen adsorption atomic centers which were beneficial to Cr(VI) reduction. Moreover, the possible reduction pathway of Cr(VI) to Cr(III) over the urea-derived g-C3N4 was proposed and the reduction process was mainly initiated by a direct reduction of photogenerated electrons.  相似文献   

12.
Polypyrrole-modified graphitic carbon nitride composites (PPy/g-C3N4) are fabricated using an in-situ polymerization method to improve the visible light photocatalytic activity of g-C3N4. The PPy/g-C3N4 is applied to the photocatalytic degradation of methylene blue (MB) under visible light irradiation. Various characterization techniques are employed to investigate the relationship between the structural properties and photoactivities of the as-prepared composites. Results show that the specific surface area of the PPy/g-C3N4 composites increases upon assembly of the amorphous PPy nanoparticles on the g-C3N4 surface. Owing to the strong conductivity, the PPy can be used as a transition channel for electrons to move onto the g-C3N4 surface, thus inhibiting the recombination of photogenerated carriers of g-C3N4 and improving the photocatalytic performance. The elevated light adsorption of PPy/g-C3N4 composites is attributed to the strong absorption coefficient of PPy. The composite containing 0.75 wt% PPy exhibits a photocatalytic efficiency that is 3 times higher than that of g-C3N4 in 2 h. Moreover, the degradation kinetics follow a pseudo-first-order model. A detailed photocatalytic mechanism is proposed with ·OH and ·O2? radicals as the main reactive species. The present work provides new insights into the mechanistic understanding of PPy in PPy/g-C3N4 composites for environmental applications.  相似文献   

13.
为了进一步提高聚合物半导体类石墨相氮化碳(g-C3N4)降解有机物的活性,通过简单的水热法复合得到碳化MoS2/掺硫g-C3N4异质结(MoSC/S-CN),并在可见光下研究其罗丹明B (RhB)的降解性能。结果表明,相较于纯g-C3N4,最优化的MoSC/S-CN样品对可见光的吸收范围得到明显拓宽,并且在100 min内对RhB的降解效率为92.5%,比纯g-C3N4性能提高68.83%。一系列的结构和光学性质表明,掺硫后再进一步与碳化MoS2耦合可以协同作用于g-C3N4,改善g-C3N4的能带结构,加速光生电子空穴对的分离,有效提高光催化活性。  相似文献   

14.
Exfoliation of bulk graphitic carbon nitride (g-C3N4) into two-dimensional (2D) nanosheets is one of the effective strategies to improve its photocatalytic properties so that the 2D g-C3N4 nanosheets (CN) have larger specific surface areas and more reaction sites. In addition, poly-o-phenylenediamine (PoPD) can improve the electrical conductivity and photocatalytic activity of semiconductor materials. Here, the novel efficient composite PoPD/AgCl/g-C3N4 nanosheets was first synthesized by a precipitation reaction and the photoinitiated polymerization approach. The obtained photocatalysts have larger specific surface areas and could achieve better visible-light response. However, silver chloride (AgCl) is susceptible to agglomeration and photocorrosion. The PoPD/AgCl/CN composite exhibits an extremely high photocurrent density, which is three times that of CN. Obviously enhanced photocatalytic activities of PoPD/AgCl/g-C3N4 are revealed through the photodegradation of tetracycline. The stability of PoPD/AgCl/CN is demonstrated based on four cycles of experiments that reveal that the degradation rate only decreases slightly. Furthermore, ?O2? and h+ are the main active species, which are confirmed through a trapping experiment and ESR spin-trap technique. Therefore, the prepared PoPD/AgCl/CN can be considered as a stable photocatalyst, in which PoPD is added as a charge carrier and acts a photosensitive protective layer on the surface of the AgCl particles. This provides a new technology for preparing highly stable composite photocatalysts that can effectively deal with environmental issues.  相似文献   

15.
The difficulty of exposing active sites and easy recombination of photogenerated carriers have always been two critical problems restricting the photocatalytic activity of g-C3N4. Herein, a simple (NH4)2MoO4-induced one-step calcination method was successfully introduced to transform bulk g-C3N4 into g-C3N4/MoO2 composites with a large specific surface area. During the calcination, with the assistance of NH3 and water vapor produced by ammonium molybdate, the pyrolytical oxidation and depolymerization of a g-C3N4 interlayer were accelerated, finally realizing the exfoliation of the g-C3N4. Furthermore, another pyrolytical product of ammonium molybdate was transformed into MoO2 under an NH3 atmosphere, which was in situ loaded on the surface of a g-C3N4 nanosheet. Additionally, the results of photocatalytic hydrogen evolution under visible light show that the optimal g-C3N4/MoO2 composite has a high specific surface area and much improved performance, which is 4.1 times that of pure bulk g-C3N4. Such performance improvement can be attributed to the full exposure of active sites and the formation of abundant heterojunctions. However, with an increasing feed amount of ammonium molybdate, the oxidation degree of g-C3N4 was enhanced, which would widen the band gap of g-C3N4, leading to a weaker response ability to visible light. The present strategy will provide a new idea for the simple realization of exfoliation and constructing a heterojunction for g-C3N4 simultaneously.  相似文献   

16.
Ag3PO4/g-C3N4 heterojunctions, with different g-C3N4 dosages, were synthesized using an in situ deposition method, and the photocatalytic performance of g-C3N4/Ag3PO4 heterojunctions was studied under simulated sunlight conditions. The results revealed that Ag3PO4/g-C3N4 exhibited excellent photocatalytic degradation activity for rhodamine B (Rh B) and phenol under the same light conditions. When the dosage of g-C3N4 was 30%, the degradation rate of Rh B at 9 min and phenol at 30 min was found to be 99.4% and 97.3%, respectively. After five cycles of the degradation experiment for Rh B, g-C3N4/Ag3PO4 still demonstrated stable photodegradation characteristics. The significant improvement in the photocatalytic activity and stability of g-C3N4/Ag3PO4 was attributed to the rapid charge separation between g-C3N4 and Ag3PO4 during the Z-scheme charge transfer and recombination process.  相似文献   

17.
In this article, novel Ag–ZnO/g-C3N4/GO ternary nanocomposites were prepared via co-precipitation method by 1%w Ag, 50% w g-C3N4, 10% w GO concentration and applied in dynamic membranes. The characteristics of Ag–ZnO/g-C3N4/GO nanocomposite were evaluated by various techniques such as X-ray diffraction, field emission scanning electron microscopy, energy dispersive X-ray map, transmission electron microscopy, X-ray photoelectron spectroscopy, photocatalyst. The photocatalytic degradation of methylene blue was investigated under visible light. The photocatalytic efficiency of 93.43% for methylene blue degradation was obtained for Ag–ZnO/g-C3N4/GO nanocomposite after 50 min of irradiation, which was remarkably higher than that of pure ZnO, bare g-C3N4, Ag–ZnO, and Ag–ZnO/g-C3N4 at the same irradiation time. Likewise, in self-forming and pre-coated membranes, ternary nanocomposites can play a vital role in the membrane surface properties, as well as their decolorization performance. The rejection of methylene blue was 30% in pure polyethersulfone membrane, while the photocatalytic degradation of methylene blue in Ag–ZnO/g-C3N4/GO nanocomposites was 88.46% and 98.86% after 10 and 15 min of irradiation in both self-forming and pre-coated dynamic membranes, respectively. Experimental results show that the dynamic membrane possesses a higher ability for degradation of MB in a shorter period of time than the static system.  相似文献   

18.
To increase the number of active sites and defects in TiO2 and promote rapid and efficient transfer of photogenerated charges, a g-C3N4@C-TiO2 composite photocatalyst was prepared via in situ deposition of g-C3N4 on a carbon-doped anatase TiO2 surface. The effects of carbon doping state and surface modification of g-C3N4 on the performance of g-C3N4@C-TiO2 composite photocatalysts were studied by X-ray diffraction, X-ray photoelectron spectroscopy, UV-visible diffuse-reflectance spectroscopy, transmission electron microscopy, electrochemical impedance spectroscopy, photoluminescence, and electron paramagnetic resonance. With increasing carbon doping content, the carbon doping state in TiO2 gradually changed from gap to substitution doping. Although the number of oxygen vacancies gradually increased, the degradation efficiency of g-C3N4@C-TiO2 for RhB (phenol) initially increased and subsequently decreased with increasing carbon content. The g-C3N4@10C-TiO2 sample exhibited the highest apparent reaction rate constant of 0.036 min?1 (0.039 min?1) for RhB (phenol) degradation, which was 150 (139), 6.4 (6.8), 2.3 (3), and 1.7 (2.1) times higher than that of pure TiO2, 10C-TiO2, g-C3N4, and g-C3N4@TiO2, respectively. g-C3N4 was grown in situ on the surface of C-TiO2 by surface carbon hybridization and bonding. The resultant novel g-C3N4@C-TiO2 photocatalyst exhibited direct Z-scheme heterojunctions with non-local impurity levels. The high photocatalytic activity can be attributed to the synergistic effects of the improved visible light response ability, higher photogenerated electron transfer efficiency, and redox ability arising from Z-type heterojunctions.  相似文献   

19.
采用热聚合法和水热法相结合的方法制备了g-C_3N_4/SnO_2复合光催化剂。利用XRD、SEM、TEM、FT-IR和UV-Vis DRS等多种测试手段对所得样品的物相结构、微观形貌和吸光特性等进行了表征。结果表明,异质结构复合光催化剂的最大光吸收边位置相对纯相SnO_2发生了明显的红移,并且SnO_2颗粒均匀分布于g-C_3N_4表面,其中最优组分(50%-g-C_3N_4/SnO_2)光催化降解染料罗丹明B(RhB)的效率达到了纯相g-C_3N_4的3.78倍。  相似文献   

20.
Novel visible-light-induced photocatalysts were fabricated by integration of Ag3VO4 and AgBr semiconductors with graphitic carbon nitride (g-C3N4) through a facile refluxing method. The fabricated photocatalysts were extensively characterized by XRD, EDX, SEM, TEM, FT-IR, UV–vis DRS, BET, TGA, and PL instruments. The photocatalytic performance of these samples was studied by degradations of three dye contaminants under visible-light exposure. Among the ternary photocatalysts, the g-C3N4/Ag3VO4/AgBr (10%) nanocomposite displayed the maximum activity for RhB degradation with rate constant of 1366.6 × 10−4 min−1, which is 116, 7.23, and 38.5 times as high as those of the g-C3N4, g-C3N4/AgBr (10%), and g-C3N4/Ag3VO4 (30%) photocatalysts, respectively. The effects of synthesis time and calcination temperature were also investigated and discussed. Furthermore, according to the trapping experiments, it was found that superoxide anion radicals were the predominant reactive species in this system. Finally, the ternary photocatalyst displayed superlative activity in removal of the contaminants under visible-light exposure, displaying great potential of this ternary photocatalyst for environmental remediation, because of a facile synthesis route and outstanding photocatalytic performance.  相似文献   

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