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1.
A strong red fluorescent nanocomposite, consisting of graphite-like carbon nitride nanosheets (g-C3N4 NSs) and serum albumin-capped Au nanoclusters (AuNCs), was synthesized. Dopamine (DA) can quench the red fluorescence of the nanocomposite, based on the Forster resonance energy transfer (FRET) mechanism. In this quenching process, the energy is transferred from the fluorescent g-C3N4 NSs-AuNCs to the oxidized DA quinine molecules (DA is easily oxidated to form DA quinine in air). The red fluorescence emission at 420 nm decreases dramatically and the quenching ratio (F0F)/F0 is linearly related to the concentration of DA in the range of 0.05–8.0 μmol L−1 with a detection limit of 0.018 μmol L−1 (S/N = 3). Additionally, this sensor has a potential of application to assay the DA in the real samples, such as human serum and human urine.  相似文献   

2.
《中国化学快报》2020,31(10):2725-2729
The porous g-C3N4 (PCN) nanosheets are successfully synthesized and further modified with nano-sized Ag by a simple wet-chemical process. Interestingly, the Ag-modified porous g-C3N4 (Ag-PCN) nanosheets exhibit competitive fluorescence detection performance of chloride ion (Cl) in aqueous solution. Under the optimized conditions, the concentration of Cl could be quantitative analyzed with the Ag-PCN in a wide detection range from 0.5 mmol/L to 0.1 mol/L, with a low detection limitation of 0.06 mmol/L. It is confirmed that the fluorescence of PCN could be effectively decayed by the photoinduced charge transfer via the adsorbed Cl for trapping holes, mainly by means of the time-resolved fluorescence and surface photovoltage spectra. The porous structure and modified Ag promote the adsorption of Cl on resulting Ag-PCN, leading to excellent fluorescence detection for Cl. This work provides a feasible route to develop a fluorescence detection of Cl with g-C3N4 nanosheets in environment water.  相似文献   

3.
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   

4.
《中国化学快报》2019,30(12):2186-2190
Graphitic carbon nitride (g-C3N4), as a visible-light-active organic semiconductor, has attracted growing attentions in photocatalysis and photoluminescence-based biosensing. Here, we demonstrated the intrinsic photooxidase activity of g-C3N4 and then surface molecular imprinting on g-C3N4 nanozymes was achieved for improved biosensing. Upon blue LED irradiation, the g-C3N4 exhibited superior enzymatic activity for oxidation of chromogenic substrate like 3,3′,5,5′-tetramethylbenzidine (TMB) without destructive H2O2. The oxidation was mainly ascribed to O2 that was generated during light irradiation. The surface molecular imprinting on g-C3N4 can lead to an over 1000-fold alleviation in matrix-interference from serum samples, 4-fold improved enzymatic activity as well as enhanced substrate specificity comparing with bare g-C3N4 during colorimetric sensing. Also, the MIP-g-C3N4 possesses a high affinity to TMB with a Km value of only 22 μmol/L, much lower than other comment nanozymes like AuNPs, Fe3O4 NPs, etc. It was successfully applied for detection of cysteine in serum sample with satisfactory recoveries.  相似文献   

5.
PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g–1 h–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g–1 h–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.  相似文献   

6.
《中国化学快报》2020,31(10):2747-2751
Graphitic carbon nitride (g-C3N4)-based materials are regarded as one of the most potential photocatalysts for utilizing solar energy. In this work, we reported a facile one step in-situ hydrothermal-roasting method for preparing honeycomb-like g-C3N4/CeO2 nanosheets with abundant oxygen vacancies (g-C3N4/CeO2-x). The hydrothermal-roasting and incomplete-sealed state can (i) generate an in-situ reducing atmosphere (CO, N2, NH3) to tune the concentration of oxygen vacancies in CeO2; (ii) beneficial to prevent continuous growth of g-C3N4 and results in honeycomb-like g-C3N4/CeO2-x hybrid nanosheets. What is more, the g-C3N4/CeO2-x photocatalyst exhibited extended photoresponse range, increased specific surface area and obviously enhanced separation efficiency of photogenerated electron-hole pairs. As a proof-of-concept application, the optimized g-C3N4/CeO2-x nanosheets could achieve 98% removal efficiency for Cr(VI) under visible light irradiation (λ ≥ 420 nm) within 2.5 h, which is significantly better than those of pure g-C3N4 and CeO2. This work provides a new idea for more rationally designing and constructing g-C3N4-based catalysts for efficient extended photochemical application.  相似文献   

7.
A novel GO modified g-C3N4 nanosheets/flower-like BiOBr hybrid photocatalyst is fabricated by a facile method. The characterization results reveal that wrinkled GO is deposited between g-C3N4 nanosheets and flower-like BiOBr forming a Z-scheme heterojunction. As a mediator, plicate GO plays a positive role in prompting photogenerated electrons transferring through its sizeable 2D/2D contact surface area. The g-C3N4/GO/BiOBr hybrid displays a superior photocatalytic ability to g-C3N4 and BiOBr in photodegrading tetracycline (TC), whose removal efficiency could reach 96% within 2 h. Besides, g-C3N4/GO/BiOBr composite can reduce Cr(VI), and simultaneously treat TC and Cr(VI) combination contaminant under the visible light. The g-C3N4/GO/BiOBr ternary composite also exhibits satisfactory stability and reusability after four cycling experiments. Further, a feasible mechanism related to the photocatalytic process of g-C3N4/GO/BiOBr is put forward. This study offers a ternary hybrid photocatalyst with eco-friendliness and hopeful application in water pollution.  相似文献   

8.
The facilitation of charge transport toward the targeted chemical reaction is a challenging task for two-dimensional (2D) nanomaterials. We demonstrate the effectiveness of two different strategies, non-metal doping and heterojunction formation, to adjust the electronic and molecular structures of g-C3N4 nanosheets (CN), which could widen the visible-light response and improve the photo-induced electron–hole separation. The g-C3N4 nanosheets containing impurity levels (boron doping (BCN)) were prepared by a high-temperature solid-state reaction. Additionally, by anchoring the 3D dichalcogenide structures (CdIn2S4) elicited by a wet chemical route, hybrid BCN/CdIn2S4 nanostructures were obtained. The resulting BCN/CdIn2S4 (BCN–CIS3) nanostructures exhibited an excellent degradation efficiency (95%) for methyl orange (MO) compared to pristine g-C3N4 nanosheets (CN) (28%) and boron-doped g-C3N4 (BCN) (35%). All the optimized photocatalysts were thoroughly characterized using various techniques and investigated for comparative structural, optical, morphological, and catalytic properties. Our results reveal that introducing boron atoms into the lattice of g-C3N4 nanosheets leads to reduction in the band-gap energy and rapid electron transfer. The formation of heterojunctions with the 3D CdIn2S4 further assists in improving the degradation efficiency by minimizing the undesired electron–hole recombination, as confirmed by time-resolved photoluminescence (TRPL) analysis. This work proposes feasible strategies and their synergy to develop innovative materials for sustainable energy conversion and environmental remediation applications.  相似文献   

9.
采用溶液中等离子放电法制备出了Pt纳米颗粒,用热氧化刻蚀和水热法成功的对石墨相氮化碳(g-C_3N_4)进行处理进而均匀吸附在科琴黑(KB)表面,最终制备出了Pt/g-C_3N_4/KB纳米复合催化剂。通过XRD分析,扫描电镜,透射电镜和电化学工作站探究了催化剂的组成、结构、颗粒大小以及电化学性能。Pt/g-C_3N_4/KB纳米复合催化剂展现出了良好的甲醇电氧化性能,性能的提升可能是由于g-C_3N_4良好的化学稳定性,N元素的存在改变Pt外层电子结构从而提高催化活性,这些因素提高了Pt的催化效率。  相似文献   

10.
采用溶液中等离子放电法制备出了Pt纳米颗粒,用热氧化刻蚀和水热法成功的对石墨相氮化碳(g-C3N4)进行处理进而均匀吸附在科琴黑(KB)表面,最终制备出了Pt/g-C3N4/KB纳米复合催化剂。通过XRD分析,扫描电镜,透射电镜和电化学工作站探究了催化剂的组成、结构、颗粒大小以及电化学性能。Pt/g-C3N4/KB纳米复合催化剂展现出了良好的甲醇电氧化性能,性能的提升可能是由于g-C3N4良好的化学稳定性,N元素的存在改变Pt外层电子结构从而提高催化活性,这些因素提高了Pt的催化效率。  相似文献   

11.
Mechanism research of nanozymes has always been of great interest since their emergence as outstanding mimics of friable natural enzymes. An important but rarely mentioned issue in mechanism research of nanozymology is the inhibitory effect of nanozymes. And conventional nanozymes with various active sites hinder the mechanism research, while single-atom Fe–N–C nanozymes with similar active sites to natural enzymes exhibit structural advantages. Herein, we synthesized Fe single-atom nanozymes (Fe-SANs) with ultrahigh oxidase-like activity and found that a common analgesic-antipyretic drug 4-acetamidophenol (AMP) had inhibitory effects for the oxidase-like activity of Fe-SANs. We investigated the inhibitory effects in detail and demonstrated that the inhibition type was reversible mixed-inhibition with inhibition constants (Ki and ) of 0.431 mM and 0.279 mM, respectively. Furthermore, we put forward a colorimetric method for AMP detection based on nanozyme inhibition. The research on the inhibitory effects of small molecules on nanozymes expands the scope of analysis based on nanozymes and the inhibition mechanism study may offer some insight into investigating the interaction between nanozymes and inhibitors.

Inhibitory effects of paracetamol on the oxidase-like activity of Fe single-atom nanozymes.  相似文献   

12.
《中国化学快报》2023,34(11):108306
Graphitic carbon nitride (g-C3N4) has been widely studied as a visible light responsive photocatalyst in recent years, due to its facile synthesis, low cost, high stability, and appropriate bandgap/band positions. In this review, we firstly introduce and compare various exfoliation approaches of bulk g-C3N4 into ultrathin g-C3N4 nanosheets. Then, many modification strategies of g-C3N4 nanosheets are also reviewed, including heterojunction construction, doping, defect control, and structure design. Thereafter, the charge transfer mechanism in g-C3N4 nanosheets based heterojunctions is present, e.g., Z-scheme, S-scheme and other forms. Besides, the photocatalytic applications of g-C3N4 nanosheets based photocatalysts are summarized including environmental remediation, energy generation and storage, organic synthesis, and disinfection. This review ends with a summary and some perspectives on the challenges and new directions in exploring g-C3N4 nanosheets-based photocatalysts.  相似文献   

13.
以合成的g-C3N4纳米片和Ag/TiO2空心微球为原料,采用机械搅拌的方法构筑了g-C3N4/Ag/TiO2三元复合光催化剂。采用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描电镜(SEM)、X射线光电子能谱(XPS)、紫外-可见光漫反射(UV-Vis DRS)和光致发光光谱(PL)对g-C3N4/Ag/TiO2进行了表征。研究表明,g-C3N4/Ag/TiO2是由Ag/TiO2微球和g-C3N4纳米片复合而成的。与TiO2相比,其可见光响应范围延长,光生载流子的分离速率加快。在室温下,用降解罗丹明B的反应考察了g-C3N4/Ag/TiO2的可见光催化活性。研究表明,光照180 min时,g-C3N4(0.5%)/Ag/TiO2显示了最高的光催化活性(91.9%),分别是TiO2和Ag/TiO2的7.5和1.8倍。光催化活性的提高与合理的异质结构建和Ag的导电性能有关。  相似文献   

14.
Although peroxidase-like nanozymes have made great progress in bioanalysis,few current nanozymebased biosensors are constructed for discriminating isomers of organic compounds.Herein,fluorescent metal-organic framework(MOF)-based nanozyme is utilized for phenylenediamine isomers discrimination and detection.NH2-MIL-101(Fe),as a member of Fe-based MOFs,functions as not only fluorescent indicator but also peroxidase mimics.In the presence of H2 O2,NH2-MIL-101(Fe) c...  相似文献   

15.
Here, we show, for the first time, the use of graphitic carbon nitride (g-C3N4) nanosheets to improve the resolution and efficiency of protein separation in gel electrophoresis. By loading 0.04% (m/v) g-C3N4 nanosheets into the polyacrylamide gel at 25 °C, the thermal conductivity increased approximately 80% which resulted in 20% reduction in Joule heating and overall increase of separation efficiency. Also, polymerization of acrylamide occurred in the absence of tetramethylethylenediamine (TEMED) when the polyacrylamide gel contained g-C3N4 nanosheets. Hence, the g-C3N4 act simultaneously as a polymerization catalyst as well as heat sinks to lower Joule heating effect on band broadening.  相似文献   

16.
Gold (Au) plasmonic nanoparticles were grown evenly on monolayer graphitic carbon nitride (g-C3N4) nanosheets via a facile oil-bath method. The photocatalytic activity of the Au/monolayer g-C3N4 composites under visible light was evaluated by photocatalytic hydrogen evolution and environmental treatment. All of the Au/monolayer g-C3N4 composites showed better photocatalytic performance than that of monolayer g-C3N4 and the 1% Au/monolayer g-C3N4 composite displayed the highest photocatalytic hydrogen evolution rate of the samples. The remarkable photocatalytic activity was attributed largely to the successful introduction of Au plasmonic nanoparticles, which led to the surface plasmon resonance (SPR) effect. The SPR effect enhanced the efficiency of light harvesting and induced an efficient hot electron transfer process. The hot electrons were injected from the Au plasmonic nanoparticles into the conduction band of monolayer g-C3N4. Thus, the Au/monolayer g-C3N4 composites possessed higher migration and separation efficiencies and lower recombination probability of photogenerated electron-hole pairs than those of monolayer g-C3N4. A photocatalytic mechanism for the composites was also proposed.  相似文献   

17.
Herein, cobalt (Co)-based metal–organic zeolitic imidazole frameworks (ZIF-67) coupled with g-C3N4 nanosheets synthesized via a simple microwave irradiation method. SEM, TEM and HR-TEM results showed that ZIF-67 were uniformly dispersed on g-C3N4 surfaces and had a rhombic dodecahedron shape. The photocatalytic properties of g-C3N4/ZIF-67 nanocomposite were evaluated by photocatalytic dye degradation of crystal violet (CV), 4-chlorophenol (4-CP) and photocatalytic hydrogen (H2) production. In presence of visible light illumination, the photocatalytic dye results showed that 95% CV degradation and 53% 4-CP degradation within 80 min. The H2 production of the g-C3N4/ZIF-67 composite was 2084 μmol g−1, which is 3.84 folds greater than that of bare g-C3N4 (541 μmol g−1).  相似文献   

18.
Two-dimensional (2D) graphitic carbon nitride (g-C3N4) nanosheets show brilliant application potential in numerous fields. Herein, a membrane with artificial nanopores and self-supporting spacers was fabricated by assembly of 2D g-C3N4 nanosheets in a stack with elaborate structures. In water purification the g-C3N4 membrane shows a better separation performance than commercial membranes. The g-C3N4 membrane has a water permeance of 29 L m−2 h−1 bar−1 and a rejection rate of 87 % for 3 nm molecules with a membrane thickness of 160 nm. The artificial nanopores in the g-C3N4 nanosheets and the spacers between the partially exfoliated g-C3N4 nanosheets provide nanochannels for water transport while bigger molecules are retained. The self-supported nanochannels in the g-C3N4 membrane are very stable and rigid enough to resist environmental challenges, such as changes to pH and pressure conditions. Permeation experiments and molecular dynamics simulations indicate that a novel nanofluidics phenomenon takes place, whereby water transport through the g-C3N4 nanosheet membrane occurs with ultralow friction. The findings provide new understanding of fluidics in nanochannels and illuminate a fabrication method by which rigid nanochannels may be obtained for applications in complex or harsh environments.  相似文献   

19.
利用g-C3N4纳米片表面的氨基与膜基底材料氯甲基化聚醚砜(CMPES)的苄氯基团发生化学交联反应,再通过相转化法制备出g-C3N4/CMPES复合膜。系统研究了g-C3N4纳米片的添加对复合膜的结构、形貌及过滤、光催化、抗污染性能的影响,并探讨其光催化降解牛血清白蛋白溶液(BSA)的机理。研究结果表明:g-C3N4纳米片与膜基底材料通过化学键相连接,有效提高了复合膜的光催化性能和稳定性。由于g-C3N4纳米片的亲水性和光催化作用,使复合膜表现出优异的过滤性能和抗污染性能。  相似文献   

20.
Bimetallic AgPd nanoparticles have been synthesized before, but the interfacial electronic effects of AgPd on the photocatalytic performance have been investigated less. In this work, the results of hydrogen evolution suggest that the bimetallic AgPd/g-C3N4 sample has superior activity to Ag/g-C3N4 and Pd/g-C3N4 photocatalysts. The UV/Vis diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, CO adsorption diffuse reflectance FTIR spectroscopy, and FTIR results demonstrate that in the AgPd/g-C3N4, the surface electronic structures of Pd and Ag are changed, which is beneficial for faster photogenerated electron transfer and greater H2O molecule adsorption. In situ ESR spectra suggest that, under visible light irradiation, there is more H2O dissociation to radical species on the AgPd/g-C3N4 photocatalyst. Furthermore, DFT calculations confirm the interfacial electronic effects of AgPd/g-C3N4, that is, Pdδ−⋅⋅⋅Agδ+, and the activation energy of H2O molecule dissociation on AgPd/g-C3N4 is the lowest, which is the main contributor to the enhanced photocatalytic H2 evolution.  相似文献   

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