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1.
The solid acid catalyst, N–F codoped TiO2/SiO2 composite oxide was prepared by a sol–gel method using NH4F as nitrogen and fluorine source. The prepared materials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), UV–Visible diffuse reflectance spectroscopy (UV–Vis), ammonia adsorption and temperature-programmed desorption (NH3-TPD), in situ Fourier transform infrared spectroscopy (FT-IR) and N2 physical adsorption isotherm. The photocatalytic activity of the catalyst for acrylonitrile degradation was investigated under simulant solar irradiation. The results showed that strong Lewis and Brønsted acid sites appear on the surface of the sample after N–F doping. Systematic investigation showed that the highest photocatalytic activity for acrylonitrile degradation was obtained for samples calcined at 450°C with molar ratio (NH4F to Ti) of 0.8. The degradation ratio of 71.5% was achieved with the prepared catalyst after 6-min irradiation, demonstrating the effectiveness of photocatalytic degradation of acrylonitrile with N–F codoped TiO2/SiO2 composite oxide. The photocatalyst is promising for application under solar light irradiation. Moreover, the intermediates generated after irradiation were verified by gas chromatography–mass spectrometry (GC–MS) analysis and UV–Vis spectroscopy to be simple organic acids with lower toxicity, and the degradation pathway was also proposed for acrylonitrile degradation with the prepared catalyst.  相似文献   

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3.
A series of cobalt doped TiO_2(Co-TiO_2) and Co Oxloaded TiO_2(Co/TiO_2) catalysts prepared by sol–gel and impregnation methods respectively were investigated on selective catalytic reduction with NH_3(NH_3-SCR) of NO. It was found that Co-TiO_2 catalyst showed more preferable catalytic activity at low temperature range. From characterization results of XRD,TEM, Raman and FT-IR, Co species were proved to be doped into TiO_2 lattice by replaced Ti atoms. After being characterized and analyzed by NH_3-TPD, PL, XPS, EPR and DRIFTS, it was found that the better NH_3-SCR activities of Co-TiO_2 catalysts, compared with Co/TiO_2 catalyst, were ascribed to the formation of more oxygen vacancies which further promoted the production of more superoxide ions(O-2). The superoxide ions were crucial for the formation of low temperature SCR reaction intermediates(NO-3) by reacting with adsorbed NO molecule. Therefore, these aspects were responsible for the higher low temperature NH_3-SCR activity of Co-TiO_2 catalysts.  相似文献   

4.
Experiments were conducted in a fixed-bed reactor containing a commercial V2O5/WO3/TiO2 catalyst to investigate mercury oxidation in the presence of HCl and O2. Mercury oxidation was improved significantly in the presence of HCl and O2, and the Hg0 oxidation efficiencies decreased slowly as the temperature increased from 200 to 400°C. Upon pretreatment with HCl and O2 at 350°C, the catalyst demonstrated higher catalytic activity for Hg0 oxidation. Notably, the effect of pretreatment with HCl alone was not obvious. For the catalyst treated with HCl and O2, better performance was observed with lower reaction temperatures. The results showed that both HCl and Hg0 were first adsorbed onto the catalyst and then reacted with O2 following its adsorption, which indicates that the oxidation of Hg0 over the commercial catalyst followed the Langmuir–Hinshelwood mechanism. Several characterization techniques, including Hg0 temperature-programmed desorption (Hg-TPD) and X-ray photoelectron spectroscopy (XPS), were employed in this work. Hg-TPD profiles showed that weakly adsorbed mercury species were converted to strongly bound species in the presence of HCl and O2. XPS patterns indicated that new chemisorbed oxygen species were formed by the adsorption of HCl, which consequently facilitated the oxidation of mercury.  相似文献   

5.
A series of CeO_2–ZrO_2–WO_3(CZW)catalysts prepared by a hydrothermal synthesis method showed excellent catalytic activity for selective catalytic reduction(SCR)of NO with NH_3 over a wide temperature of 150–550°C.The effect of hydrothermal treatment of CZW catalysts on SCR activity was investigated in the presence of 10% H_2O.The fresh catalyst showed above 90% NO_x conversion at 201–459°C,which is applicable to diesel exhaust NO_x purification(200–440°C).The SCR activity results indicated that hydrothermal aging decreased the SCR activity of CZW at low temperatures(below 300°C),while the activity was notably enhanced at high temperature(above 450°C).The aged CZW catalyst(hydrothermal aging at 700°C for 8 hr)showed almost 80% NO_x conversion at 229–550°C,while the V_2O_5–WO_3/TiO_2 catalyst presented above 80% NO_x conversion at 308–370°C.The effect of structural changes,acidity,and redox properties of CZW on the SCR activity was investigated.The results indicated that the excellent hydrothermal stability of CZW was mainly due to the CeO_2–ZrO_2 solid solution,amorphous WO_3 phase and optimal acidity.In addition,the formation of WO_3 clusters increased in size as the hydrothermal aging temperature increased,resulting in the collapse of structure,which could further affect the acidity and redox properties.  相似文献   

6.
Resource recycling from waste-water and sludge is an important part of the 14th Five-Year Plan in China. The emerging titanium-based coagulants have drawn growing attentions due to their strong coagulation capability in water purification and value-added Ti-loaded sludge production. Management and recovery of the high value-added sludge into functional nanomaterials is highly significant for both sludge reduction and environmental remediation.The present study was carried out to investigate the ...  相似文献   

7.
Introduction N um erous studies have utilized a strong oxidizing pow der of TiO 2 photocatalysts to degrade aqueous or gaseous toxic organic pollutants for w ater purification, w astew ater treatm ent and air pollution control (Fujishim a et al., 2001; K …  相似文献   

8.
Developing low-temperature SO2-tolerant catalysts for the selective catalytic reduction of NOx is still a challenging task. The sulfation of active metal oxides and deposition of ammonium bisulfate deactivate catalysts, due to the difficult decomposition of the as-formed sulfate species at low temperatures(<300 °C). In recent years, metal sulfate catalysts have attracted increasing attention owing to their good catalytic activity and strong SO2 tolerance at hi...  相似文献   

9.
TiO_2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface water, we herein examined the preparation of a P25-TiO_2 composite film on a cement substrate via a sol–gel method. In this case, Rhodamine B(Rh B)was employed as the target organic pollutant. The self-generated TiO_2 film and the P25-TiO_2 composite film were characterized by X-ray diffraction(XRD), N_2 adsorption/desorption measurements, scanning electron microscopy(SEM), transmission electron microscopy(TEM), and diffuse reflectance spectroscopy(DRS). The photodegradation efficiencies of the two films were studied by Rh B removal in water under UV(ultraviolet) irradiation. Over 4 day exposure, the P25-TiO_2 composite film exhibited higher photocatalytic performance than the self-generated TiO_2 film. The photodegradation rate indicated that the efficiency of the P25-TiO_2 composite film was enhanced by the addition of the rutile phase Degussa P25 powder. As such, cooperation between the anatase TiO_2 and rutile P25 nanoparticles was beneficial for separation of the photo-induced electrons and holes. In addition, the influence of P25 doping on the P25-TiO_2 composite films was evaluated. We found that up to a certain saturation point, increased doping enhanced the photodegradation ability of the composite film. Thus, we herein demonstrated that the doping of P25 powders is a simple but effective strategy to prepare a P25-TiO_2 composite film on a cement substrate, and the resulting film exhibits excellent removal efficiency in the degradation of organic pollutants.  相似文献   

10.
目的研究层涂法制备Pr~(3+):Y_2SiO_5/TiO_2复合薄膜的结构与可见光催化性能。方法分别以钛酸丁酯(TBOT)和正硅酸乙酯(TEOS)为前驱体,通过溶胶-凝胶法制得TiO_2凝胶和Pr掺杂的Y_2SiO_5凝胶,以碳纤维为薄膜载体,并通过浸渍提拉法制备Pr~(3+):Y_2SiO_5/TiO_2层涂薄膜,研究层涂法制备复合薄膜对复合薄膜结构、形貌以及光催化效果的影响。结果复合薄膜具有明显的分层界限,形貌较平整,有较少龟裂;复合薄膜性能受涂覆次序的影响较大。结论依次将Pr~(3+):Y_2SiO_5和TiO_2涂覆在碳纤维上的复合薄膜具有较好的光催化性能,可见光光照2 h,对亚甲基蓝的脱色率达到94%,其可见光催化效率高于TiO_2薄膜的59%。  相似文献   

11.
This work shows the synthesis,characterization and evaluation of dense-ceramic membranes made of Ce0.85Gd0.15O2-δ-LaNiO3(CG-LN) composites,where the fluorite-perovskite ratio (CG:LN) was varied as follows:75:25,80:20 and 85:15 wt.%.Supports were initially characterized by XRD,SEM and electrical conductivity (using vacuum and oxygen atmospheres),to determine the composition,microstructural and ionic-electronic conductivity properties.Later,supports were...  相似文献   

12.
It remains as a challenge for realizing efficient photo-responsive catalysts towards largescale degradation of organic pollutants under natural sunlight.This work reports a new pore engineering strategy for creating ultra-porous g-C3N4 micro-tubes with an unprecedentedly high specific surface area of 152.96 m2/g.This is mainly associated with releasing internal vapor pressure in the autoclave where the hydrothermal treatment of the urea/melamine mixture is proces...  相似文献   

13.
Experiments were conducted in a fixed-bed reactor that contained a commercial catalyst, V2O5–WO3/TiO2, to investigate mercury oxidation in the presence of NO and O2. Mercury oxidation was improved by NO, and the efficiency was increased by simultaneously adding NO and O2. With NO and O2 pretreatment at 350°C, the catalyst exhibited higher catalytic activity for Hg0 oxidation, whereas NO pretreatment did not exert a noticeable effect. Decreasing the reaction temperature boosted the performance of the catalyst treated with NO and O2. Although NO promoted Hg0 oxidation at the very beginning, excessive NO counteracted this effect. The results show that NO plays different roles in Hg0 oxidation; NO in the gaseous phase may directly react with the adsorbed Hg0, but excessive NO hinders Hg0 adsorption. The adsorbed NO was converted into active nitrogen species (e.g., NO2) with oxygen, which facilitated the adsorption and oxidation of Hg0. Hg0 was oxidized by NO mainly by the Eley–Rideal mechanism. The Hg0 temperature-programmed desorption experiment showed that weakly adsorbed mercury species were converted to strongly bound ones in the presence of NO and O2.  相似文献   

14.
An innovative photoelectrode, B2O3·TiO2/Ti electrode, was prepared by galvanostaticanodisation. The morphology and crystalline texture of the B2O3·TiO2 film on electrode were examined by acomic force microscopy (AFM) and X-ray diffraction respectively. The examination results indicated that the anatase was the dominant component. The kinetics of photoelectrocatalytic(PEC) degradation of humic acid(HA) was investigated; the results demonstrated that effects from strongness to weakness on the photoelectrocatalytic degraded rate of humic acid: power of UV-lamp, area of TiO2 film, bias, original concentration of humic acid solution. The optimum conditions were power of UV-lamp 125 W, area of TiO2 film 42.0 cm2 , bias 1.4 V, original concentration of humic acid solution 5 mg/L in this PEC reaction system.  相似文献   

15.
High-efficiency photocatalysts are of great significance for the application of photocatalytic technology in water treatment.In this study,N/Cu co-doped ZnS nanosphere photocatalys(N/Cu-ZnS) is synthesized by a hydrothermal method for the first time.After doping,the tex ture of nanosphere becomes loose,the nanometer diameter is reduced,making the specific surface area of catalyst increased from 34.73 to 101.59 m2/g.The characterization results show that more ZnS (111) crystal planes a...  相似文献   

16.
The photochemical reaction of14CS 2 with OH has been studied.The results indicated that the main products of the reaction were14COS and 14CO with a small amount of 14CO2 in the reaction system(14CS2-H2O2-C3H8-N2-O2>).The reaction was promoted by oxygen.14COS and 14CO had the similar kinetic curves while 14CO2 got a different kind of Curve.The overall rate constant increased with the increasing of oxygen partial pressure.The rate constant for the removal of 14CS2 was K=3.4×10-12cm3/(mO1.s) at 33330 Pa 02.The conversion of 14CS2 to 14CO2 at room temperature was observed and the possible mechanism of the photochemical reaction was disscussed.  相似文献   

17.
AdiagnosticexperimentoftheinfluenceofCO_2onwinterwheatWangChunyi;BaiYueming;WenMin(ChineseAcadernyofMeteorologicalSciences,Be...  相似文献   

18.
The photocatalytic oxidation of gaseous chlorobenzene(CB) by the 365 nm-induced photocatalyst La/N–Ti O2, synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology(RSM) was used to model and optimize the conditions for synthesis of the photocatalyst. The optimal photocatalyst was 1.2La/0.5N–Ti O2(0.5) and the effects of La/N on crystalline structure, particle morphology, surface element content, and other structural characteristics were investigated by XRD(X-ray diffraction), TEM(Transmission Electron Microscopy), FTIR(Fourier transform infrared spectroscopy), UV–vis(Ultraviolet–visible spectroscopy), and BET(Brunauer Emmett Teller). Greater surface area and smaller particle size were produced with the co-doped Ti O2 nanotubes than with reference Ti O2. The removal of CB was effective when performed using the synthesized photocatalyst,though it was less efficient at higher initial CB concentrations. Various modified Langmuir-Hinshelwood kinetic models involving the adsorption of chlorobenzene and water on different active sites were evaluated. Fitting results suggested that competitive adsorption caused by water molecules could not be neglected, especially for environments with high relative humidity. The reaction intermediates found after GC–MS(Gas chromatography–mass spectrometry) analysis indicated that most were soluble, low-toxicity, or both. The results demonstrated that the prepared photocatalyst had high activity for VOC(volatile organic compounds) conversion and may be used as a pretreatment prior to biopurification.  相似文献   

19.
Heterogeneous photocatalytic degradation of γ-HCH on soil surfaces was carded out to evaluate the photocatalytic effectiveness of α-Fe2O3 and TiO2 toward degrading γ-HCH on soil surfaces. After being spiked with γ-HCH, soil samples were loaded with α-Fe2O3 or TiO2 and exposed to UV-light irradiation. Different catalyst loads, 0%, 2%, 5%, 7%, and 10% (wt.)α-Fe2O3 ; 0%, 0.5%, 1%, 2:(Wt.)TiO2, were tested for up to 7 d irradiation. The effects of soil thickness, acidity, and humic substances were also investigated. The obtained results indicated that the γ-HCH photodegradation follows the pseudo-first-order kinetics. The addition of α-Fe2O3 or TiO2 accelerates the photodegradation of γ-HCH, while the photodegradation rate decreases when the content of α-Fe2O3 exceeds 7% (wt.).The degradation rate increases with the soil pH value. Humic substances inhibit the photocatalytic degradation of γ-HCH., and trichlorobenzene are detected as photodegradation intermediates, which are gradually degraded with the photodegradation evolution.  相似文献   

20.
Nonylphenol(NP) residues, as a typical endocrine disrupting chemical(EDC), frequently exist in sewage, surface water, groundwater and even drinking water, which poses a serious threat to human health due to its bioaccumulation. In order to remove NP, a series of MIL-100(Fe)/Zn Fe2O4/flake-like porous carbon nitride(MIL/ZC) was synthesized through in-situ synthesis at room temperature. High performance of ternary MIL/ZC is used to degrade NP under visible light irradiation. ...  相似文献   

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