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1.
《Advanced Powder Technology》2020,31(5):1891-1902
The one-pot synthesis of g-C3N4-MU isotype heterojunction has been produced by the thermal polycondensation method by mixing different ratios of precursors between melamine and urea. The isotype heterojunction g-C3N4-MU samples were characterized by X-ray diffraction spectroscopy, scanning electron microscope and energy-dispersive X-ray-spectroscopy, UV–Visible diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy. The band-gap energy of these photocatalysts reveals that they can work well under visible light. The photocatalytic performance of the samples was investigated over the photodegradation of reactive orange-16 (RO-16) dye and tetracycline hydrochloride (TC-HCl) under visible light irradiation. The isotype heterojunction of g-C3N4-M6U10 showed the highest degradation of 95 and 85.6% for RO-16 and TC-HCl, respectively under irradiation time of 100 and 120 min. The major reactive species was identified as O2. Moreover, the reusability of the photocatalyst was investigated up to 3 cycles with good efficiency. The present synthesized isotype heterojunction g-C3N4-MU could be applied as a facile pathway for synthesis and as an effective pathway to resolve various environmental problems.  相似文献   

2.
《Advanced Powder Technology》2020,31(7):2921-2931
The hybrid graphitic carbon nitride-cadmium oxide (g-C3N4/CdO) nanocomposite was fabricated using chemical precipitation and self-assembly method. The photocatalysts were characterised by XRD, XPS, FTIR, BET, TEM, FESEM, UV-Vis and PL spectroscopy. Based on the optical study, visible light harvesting was improved and the band gap of bulk g-C3N4 to hybrid g-C3N4/CdO nanocomposite was greatly reduced from 2.72 eV to 2.35 eV, signifying a better charge carrier mobility. The photocatalytic activity were further assessed by conducting rhodamine B (RhB) photodegradation reaction using visible light. An excellent dye removal efficiency of 96% was achieved when 1.5 g/L of hybrid g-C3N4/CdO nanocomposite was used with an initial concentration of 10 ppm for 120 min whereas only 66% of RhB was removed by bulk g-C3N4 within the same operating conditions. Besides, reusability tests were carried out and evidenced that hybrid g-C3N4/CdO nanocomposite can be recycled up to four times by retaining the degradation efficiency. The scavenging studies confirmed that the RhB photodegradation using hybrid g-C3N4/CdO nanocomposite was controlled by valance band h+ and O2− oxidation reactions. Conclusively, the inclusion of CdO onto g-C3N4 resulted in remarkable photocatalytic activity for dye degradation applications.  相似文献   

3.
《Advanced Powder Technology》2020,31(10):4344-4353
The extensive and accumulative use of tetracycline (TC) in the environment has become a serious problem. In this study, MIL-88A/g-C3N4 micro-nano particles were successfully prepared through a simple, low-cost, one-step hydrothermal method for TC adsorption in water. At a pH of 7.0, the maximum adsorption capacity (154.51 mg·g−1) of MIL-88A/g-C3N4 is reached at room temperature. Owing to its porous structure and large pore size (>2.06 nm) of MIL-88A/g-C3N4, TC can be adsorbed on both external and internal surfaces. Kinetic and thermodynamic studies have shown that the pseudo-second-order kinetic and the Langmuir-Freundlich model can be used to describe the adsorption process, which is a spontaneous endothermic process. The mechanism study reveals that the TC adsorption process by MIL-88A/g-C3N4 is mainly through electrostatic interaction and the ion exchange of COOH and NH2 groups on MIL-88A/g-C3N4 to TC. After simple pickling and water washing, MIL-88A/g-C3N4 can still reach 83.1% of the original adsorption capacity after five cycles, which proves that MIL-88A/g-C3N4 can be a promising adsorbent.  相似文献   

4.
《Advanced Powder Technology》2021,32(12):4522-4532
Construction of heterojunction with reusability is one of the effective ways to avoid secondary pollution and strengthen photocatalysis. Herein, a magnetically recyclable Z-scheme Bi4O5I2/NiFe2O4 heterojunction photocatalyst was successfully fabricated by a two-step hydrothermal method. Through adjusting the theoretical molar proportion of NiFe2O4 to Bi4O5I2, it was verified that the optimal composite could decompose 98.5% Rhodamine B (RhB, 10 mg/L) within 60 min under simulative sunlight and 98.1% RhB within 80 min under visible light. According to the characterizations, the superior performance was mainly associated with the small band gap energy (2.44 eV) and efficient separation of photo-generated electrons and holes caused by the formation of heterojunction. Meanwhile, the enlarged specific area (27.6 m2/g) provided many adsorptive sites and active sites to improve the reaction further. Moreover, the trapping experiment indicated that the photodegradation involved O2, OH and h+. After confirming the reliable activity, reusability and stability of the photocatalyst, an inferred mechanism was shown. In summary, the design of this magnetically recyclable Z-scheme Bi4O5I2/NiFe2O4 heterojunction photocatalyst can become a new choice to purify wastewater.  相似文献   

5.
Herein, a novel CoTiO3/BiOI (CTOB) p-n heterojunction with nanosheets-on microrods structure were prepared via a simple coprecipitation method for the first time. The catalysts were carefully characterized by various instruments. The CTOB heterostructures display improved photocatalytic performance towards RhB degradation. Among CTOB composites, CTOB-15 exhibits the optimal photocatalytic performance. Moreover, CTOB-15 also shows enhanced photocatalytic activity for MO and TC degradation compared to bare catalysts. The degradation rate constants for RhB and MO by CTOB-15 heterostructure are ca 1.6 and 1.4-fold higher than bare BiOI. The improved photocatalytic performance could be on account of the efficient separation of photoinduced carriers as well as enhanced light absorbance. Trapping experiments indicates that holes (h+) and superoxide anion radical (O2) play a significant role in the removal of RhB by CTOB composites. The excellent photocatalytic activity and stability make it a promising photocatalyst in environmental remediation.  相似文献   

6.
Constructing heterojunction provides a promising tactic to improve the photocatalytic efficiency of catalysts. In this paper, hierarchical FeIn2S4/BiOBr heterostructure photocatalysts were prepared by facile two step methods and applied to effectively remove ciprofloxacin (CIP) and tetracycline (TC) under visible light. Compared to single catalyst, FeIn2S4/BiOBr hybrids display significantly improved photocatalytic activity. Among the series, 6 wt% FeIn2S4/BiOBr shows the optimal photocatalytic performance, where the degradation efficiencies of TC and CIP are 3.15 and 2.88 times greater than pure BiOBr, respectively. Such an improvement could arise from the S-scheme heterojunctions and unique hierarchical structures, which brings stronger light absorption, higher photoexcited charge separation efficiency and superior redox ability. Furthermore, 6 wt% FeIn2S4/BiOBr composite exhibits excellent stability and reusability. Radical capture experiments and EPR analyses uncover that O2, h+ and OH are primarily reactive substances during photocatalytic removal of TC. The products of TC were detected by LC-MS analyses and possible decomposition paths are proposed. Eventually, a possible photodegradation mechanism over FeIn2S4/BiOBr S-scheme heterojunction is proposed. These findings supply new perspective for the simple synthesis of S-scheme photocatalysts with promising applications in environment remediation.  相似文献   

7.
Perovskites with stable crystal structure and excellent catalytic performance have attracted extensive attention in peroxomonosulfate (PMS) activation, however, severe agglomeration has always been the main obstacle limiting the catalytic activity of them, so novel perovskite catalysts are urgently needed. In this study, three-dimensional ordered macroporous silica (3DOM SiO2) was prepared by colloidal crystal template method, then CeO2@LaMnO3/3DOM SiO2 was prepared by sol-gel method combined with impregnation method and used to activate PMS for urotropine (URO) degradation. CeO2@LaMnO3/3DOM SiO2 activated PMS system exhibited high URO removal efficiency and quick kinetic, as 99.98 % URO was degraded even within 30 min. The catalyst has a wide pH range and still has high catalytic activity in the presence of organic matter and inorganic ions. The three components in CeO2@LaMnO3/3DOM SiO2 showed a synergetic effect. CeO2 and LaMnO3 were uniformly loaded on 3DOM SiO2, which effectively avoided agglomeration. The specific surface area of CeO2@LaMnO3/3DOM SiO2 was 11.88 times that of LaMnO3 prepared by sol-gel method. There are two redox cycles of Ce3+/Ce4+ and Mn2+/Mn3+/Mn4+ in CeO2 and LaMnO3, respectively, which synergistically realize the activation of PMS. Both quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that that SO4?, OH and 1O2 jointly achieved the degradation of URO. In summary, CeO2@LaMnO3/3DOM SiO2 would be a promising candidate for practical wastewater treatment.  相似文献   

8.
《Advanced Powder Technology》2021,32(11):4210-4221
In engineering application area, it has always been a challenge to simultaneously improve flame-retardant performance and crystallization rate of polylactic acid (PLA) biomaterials, thus restricting their extensive application. In this work, a multifunctional additive (4,4′-(phenylphosphoryl)bis(piperazine-4,1-diyl))bis(diphenylphosphine oxide) (PDPO) was successfully synthesized and used to fabricate flame retardant PLA biocomposites. The crystallization behavior, fire safety, mechanical properties and flame retardant mechanisms of PLA biocomposites were studied in detail. The results indicated that PDPO notably improved the crystallization rate and crystallinity of PLA biocomposites. When 4 wt% PDPO was incorporated, PLA/PDPO biocomposites successfully passed UL-94V-0 grade and their LOI values were improved from 19.0% of pure PLA to 29.4%. The introduction of PDPO promoted the premature degradation and carbonization of PLA substrate, and inhibited the transesterification of the PLA during thermal pyrolysis process. Besides, PDPO decomposed and produced the Ph and PO, which efficiently exerted the free radical trapping effect in vapor phase. Therefore, the spread of fire for PLA/PDPO was declined and even self-extinguished. Meanwhile, the low addition of PDPO presented little effect on the mechanical properties of PLA composites. This flame retardant PLA biocomposites showed broad application prospects in emerging fields such as electronic devices, automobiles, and 3D printing materials.  相似文献   

9.
Fabrication of FeOOH@Bi2MoO6 composites was successfully carried out by the solvent thermal-impregnation method, and they were used as effective visible light-driven photo-Fenton catalysts. The catalyst can achieve effective degradation of CIP in the pH range of 3.5–10.5, which overcomes the problems of harsh pH application conditions and low H2O2 utilization in Fenton. Notably, FeOOH@Bi2MoO6 exhibited stronger photo-Fenton catalytic activity compared with pure FeOOH, pure Bi2MoO6 and their simple physical mixtures, indicating that the interfacial active sites of FeOOH and Bi2MoO6 are favorable for the rapid transfer of photogenerated electrons from Bi2MoO6 to FeOOH. Combined with the characterization analysis and performance experiments, the catalytic mechanism of the FeOOH@Bi2MoO6-H2O2 system is reasonably proposed. The photocatalytic-Fenton synergy facilitates the rapid separation of photogenerated carriers and the valence cycling of Fe(III)/Fe(II), which drives the reaction system to produce a large amount of OH, O2? and a small amount of h+ to participate in the degradation process of CIP. In this study, the preparation of composite catalysts and the coupled use of photocatalytic-Fenton provided a feasible idea to overcome the problems of narrow pH application and low H2O2 utilization in Fenton.  相似文献   

10.
《Advanced Powder Technology》2020,31(7):2618-2628
In this research, Bi4O5I2 and AgI nanoparticles were anchored over g-C3N4 nanosheets (denoted as NGCN/Bi4O5I2/AgI) to preparation highly impressive visible-light-driven samples. The synthesized nanocomposites were investigated by X-ray diffraction (XRD), Fourier transform-infrared (FT-IR), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), UV–vis diffuse reflectance spectroscopy (DRS), energy dispersive analysis of X-rays (EDX), electrochemical impedance spectroscopy (EIS), photocurrent density, Brunauer-Emmett-Teller (BET), and photoluminescence (PL) analyses. Among the ternary photocatalysts, the NGCN/Bi4O5I2/AgI (20%) photocatalyst illustrated the highest photoactivity in degradation of rhodamine B (RhB), which was approximately 58.4, 15.2, and 12.8 times higher than the GCN, NGCN, and NGCN/Bi4O5I2 (20%) samples, respectively. Furthermore, the O2 was discovered as the main species in the respective system by the quenching tests. Also, by studying the electrochemical properties, a cascade photocatalytic mechanism was suggested based on the energy bands to describe the enhanced charge carriers migration and separation, which caused impressive photocatalytic performances in degradations of four hazardous contaminants. This study highlights the rational anchoring of Bi4O5I2 and AgI nanoparticles over NGCN to prepare highly efficient photocatalysts for wastewater remediation.  相似文献   

11.
12.
《Advanced Powder Technology》2020,31(6):2327-2336
Herein, we prepare novel composites of α-Fe2O3/BiOI photocatalysts by one step microwave hydrothermal process. The SEM and TEM characterization results suggest microsphere shaped of BiOI with α-Fe2O3 nanoparticles decorated on the surface of BiOI nanosheets. According to the results of UV-vis DRS measurements, α-Fe2O3/BiOI exhibited more visible light adsorption. The composite exhibited the highest photoactivity for decomposition of methyl orange (MO) and antibiotics tetracycline (Tc) superior to that of the pure α-Fe2O3 and BiOI in the visible light. The degradation rate constant is 2.3 times and 2.0 times higher than that of pure BiOI and α-Fe2O3 under the same conditions for degradation MO and Tc respectively. The photodegradation performances of α-Fe2O3/BiOI composites were also investigated under different light sources irradiation. Based on the analysis results of radical capture experiment, the enhanced photocatalytic efficiency of α-Fe2O3/BiOI photocatalyst can be mainly indentified to be the dominant active species of hole (h+) and superoxide radical(O2).  相似文献   

13.
In this work, magnetic nanoparticles (MNPs) grafted with carboxylic acid (Fe3O4-COOH MNPs) were successfully prepared from incorporation of glutaric anhydride as a functional group on the surface of the ferrite NPs. The MNP was used as a template to induce the growth of ZIF-8 metal–organic framework (MOF) on its surface. The Fe3O4-COOH@ZIF-8 core-shell was incorporated with silver phosphate (Ag3PO4) and Ag nanoparticles (Ag NPs) to develop a visible light active Fe3O4-COOH@ZIF-8/Ag/Ag3PO4 photocatalyst. The materials were characterized using a range of techniques. The photocatalytic activity was investigated systematically by degrading an organo-phosphorus pesticide, diazinon under visible light irradiation. Among synthesized samples, the Fe3O4-COOH@ZIF-8/Ag/Ag3PO4 heterostructured system exhibited highest photocatalytic activity and improved stability compared to others for the degradation of diazinon under visible light. The superior activity and improved stability of this heterostructured photocatalyst was attributed to the synergistic effects from surface plasmon resonance (SPR) of Ag NPs and sequential energy transfer via Z-scheme mechanism, for effective separation of electron-hole pairs. Radical-trapping experiments demonstrate that holes (h+) and O2 are primary reactive species involved in photocatalytic oxidation process. Moreover, the Fe3O4-COOH@ZIF-8/Ag/Ag3PO4 photocatalyst did not show any obvious loss of photocatalytic activity during five cycle tests, which indicate that the heterostructured photocatalyst was highly stable and can be used repeatedly. Therefore, the work provides new insights into the design and fabrication of metal-organic frameworks (MOFs) for use as a visible light photocatalyst for degrading organic contaminants.  相似文献   

14.
The UiO-66-NH2 and graphene quantum dot suspension were synthesized through hydrothermal and electrochemical methods, respectively. The prepared species were assembled on a non-woven polypropylene substrate (NW-PP). The obtained microstructure and the efficiency of the assembling methods were compared to each other. The results showed that plasma treatmentof NW-PP, as the pre-treating procedure, was the most liable strategy concerning the homogenous distribuation of MOF (mass loading percentage of ~19.5 wt% of UiO-66-NH2) and improved filtering performance. Next, the photocatalytic performance against methylene blue was increased through addition of graphene quantum dot (GQD) to the NW-PP. The photoluminescence results confirmed that the presence of GQDs effectively inhibited the recombination of photogenerated electron/hole pairs. In addition, the photocatalytic constant rate was increased up to ~three times in the presence of GQDs. Quenching tests proved that the photo-generated O2? played a major role in the photodegradation of the dye.  相似文献   

15.
Small changes in a catalyst’s composition, modification, and/or integration into a reactor can have significant yet often poorly understood effects on (electro)catalysis. Here we demonstrate the careful tailoring of Ru/La0.25Ce0.75O2−x catalysts through the post-synthesized hydrothermal treatment together with control over the Ru loadings to create hydroxyl groups and electronic restructuring for ammonia electrosynthesis. When integrated into a protonic ceramic electrolyzer, the in situ formed Ce3+−OH/Ru sites facilitate both the NN decoupling and NH formation at 400 °C and 1 bar of N2, boosting the ammonia production rate (2.92 mol h−1 m−2) up to 100-fold higher than the current state-of-the-art electrolyzers. Moreover, such catalysts and electrolyzer design concepts can be readily tuned to more complex applications such as coproducing ammonia and other chemicals with hydrocarbons as direct hydrogen sources. The creation of coordinated saturated support –OH/metal sites in the advanced electrolyzer offers an attractive approach for future clean-energy and green-chemical industries.  相似文献   

16.
《材料科学技术学报》2019,35(10):2288-2296
Rationally engineering the microstructure and electronic structure of catalysts to induce high activity for versatile applications remains a challenge. Herein, chlorine doped graphitic carbon nitride (Cl-doped g-C3N4) nanorings have been designed as a superior photocatalyst for pollutant degradation and oxygen evolution reaction (OER). Remarkably, Cl-doped g-C3N4 nanorings display enhanced OER performance with a small overpotential of approximately 290 mV at current density of 10 mA cm−2 and Tafel slope of 83 mV dec-1, possessing comparable OER activity to precious metal oxides RuO2 and IrO2/C. The excellent catalytic performance of Cl-doped g-C3N4 nanorings originates from the strong oxidation capability, abundant active sites exposed and efficient charge transfer. More importantly, visible light irradiation gives rise to a prominent improvement of the OER performance, reducing the OER overpotential and Tafel slope by 140 mV and 28 mV dec-1, respectively, demonstrating the striking photo-responsive OER activity of Cl-doped g-C3N4 nanorings. The great photo-induced improvement in OER activity would be related to the efficient charge transfer and the OH radicals arising spontaneously on CN-Cl100 catalyst upon light irradiation. This work establishes Cl-doped g-C3N4 nanorings as a highly competitive metal-free candidate for photoelectrochemical energy conversion and environmental cleaning application.  相似文献   

17.
《Advanced Powder Technology》2021,32(9):3278-3287
The influence of NO2 concentration and exposure time on the degradation of polyphenylene sulfide (PPS) fabric filter at high temperature was investigated in detail. PPS fiber damage in the filter became more severe with increasing NO2 concentration and exposure time. The elastic modulus of the PPS filter increased rapidly during the initial stage of exposure, and then increased more slowly to reach an almost constant value, nearly independent of NO2 concentration. The tensile strength also decreased significantly during the initial stage, gradually attaining a constant value with increasing exposure time. Higher NO2 concentrations resulted in rapid reducing of the tensile strength. Short exposure time to lower NO2 concentrations caused the oxidation of S atoms in PPS to SO and OSO, whereas oxidation of benzene rings in PPS were induced only with longer exposure times and higher NO2 concentrations. The model proposed in our previous paper accurately expresses the change in PPS conversion and reaction rate for every NO2 concentration. An improved model that successfully estimated the degradation of tensile strength in both the machine direction and transverse direction, regardless of NO2 concentration, was also proposed.  相似文献   

18.
The reduction conversion of 4-nitroaniline (4-NA) to p-phenylenediamine (PPD) via semiconductor photocatalysis has been considered as one of the most promising technologies to satisfy the requirement of modern industrial development. In this work, Bi4NbO8Cl materials with different calcination temperatures were successfully obtained by a facile synthesis method. Attractively, Bi4NbO8Cl nanosheet was put forward to catalyze 4-nitroaniline into p-phenylenediamine (PPD), which presented an ultra-high performance for the reduction of 4-nitroaniline under visible light irradiation. The optimal Bi4NbO8Cl nanosheets without an additive of noble metal cocatalyst can achieve conversion of 4-nitroaniline into p-phenylenediamine in 5 min. Furthermore, the crystal structure, optical properties, microscopic morphology, element chemical states, and photoelectrochemical properties of these photocatalysts were systematically investigated by various physical and chemical characterizations. Thereinto, Bi4NbO8Cl material displays a uniform morphology of nanosheets, and the size of nanosheets becomes larger and larger with the increase of calcination temperature. Simultaneously, prominent durability and reproducibility were accomplished via the above-mentioned photocatalyst. In addition, the CO2? radicals acting as primary active species can be confirmed by some controlled experiments and active species trapping experiments. This work provides a high-efficiency photocatalyst for the hydrogenation of 4-nitroaniline into p-phenylenediamine (PPD), and a possible reaction mechanism was uncovered and proposed.  相似文献   

19.
“Non-firing” ceramics have recently attracted much attention in recent years because many functional materials can be achieved by this method without the aid of sintering process. Amorphous silica powder was mechanically treated by a planetary ball mill system, by which the surface of powders was activated and simultaneously particle size reduced extensively. Surface of powders with different milling conditions was investigated by scanning electron microscopy (SEM) and nitrogen adsorption isotherm. The surface activity of raw and treated silica powders was measured based on the water adsorbed volume on the powder surface. Results showed that the powder surface was activated, and the silica powders were pulverized as an effect of ball milling. At milling times as short as 15?min, the powder was rubbed against balls, and the friction between particle/ball breaks the bonds of functional groups like SiOSi on the surface of particles. For longer milling times, powders were pulverized and more new active surfaces were formed.  相似文献   

20.
《Advanced Powder Technology》2019,30(12):2881-2889
The degradation behavior of polyphenylene sulfide (PPS) fabric filter media by NO2 gas at high temperatures was investigated in detail with a continuous-flow type exposure method, as specified in ISO16891:2016. An increase in the exposure time to NO2 gas lessened the tensile strength and elongation of the PPS filter media in both machine and transverse directions. These reductions were observed in the transverse direction (TD) more markedly than in the machine direction (MD). Exposure to NO2 gas enhanced the oxidation of sulfur, and introduced new oxygen-containing functional groups (e.g., SO and OSO) into the PPS molecular structure, which reduced the atomic ratio of carbon in the PPS filter media with increasing exposure time. These chemical degradations severely damaged the PPS fiber through cracking, splitting, and formation of protrusions on the surface.Furthermore, assuming that the chemical reaction between PPS and NO2 gas is diffusion-controlled by NO2, a model to estimate the change in the conversion of PPS and the NO2 concentration in the exhaust gas was proposed, based on an unreacted core model. It could successfully reproduce the experimental data. A model to evaluate the change in the tensile strength of the filter media was also proposed, which could express experimental data only in the MD.  相似文献   

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