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1.
Ce1?x Cu x O2 oxide solid solution catalysts with different Ce/Cu mole ratios were synthesized by the one-pot complex method. The prepared Ce1?x Cu x O2 catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and H2 temperature-programmed reduction (H2-TPR). Their catalytic properties were also investigated by catalytic combustion of phenyl volatile organic compounds (PVOCs: benzene, toluene, xylene, and ethylbenzene) in air. XRD analysis confirmed that the CuO species can fully dissolve into the CeO2 lattice to form CeCu oxide solid solutions. XPS and H2-TPR results indicated that the prepared Ce1?x Cu x O2 catalysts contain abundant reactive oxygen species and superior reducibility. Furthermore, the physicochemical properties of the prepared Ce1?x Cu x O2 catalysts are affected by the Ce/Cu mole ratio. The CeCu3 catalyst with Ce/Cu mole ratio of 3.0 contains abundant reactive oxygen species and exhibits superior catalytic combustion activity of PVOCs. Moreover, the ignitability of PVOCs is also affected by the respective physicochemical properties. The catalytic combustion conversions of ethylbenzene, xylene, toluene, and benzene are 99%, 98.9%, 94.3%, and 62.8% at 205, 220, 225, and 225 °C, respectively.  相似文献   

2.
We investigated the effects of different Cu weight ratio on θ or γ-Al2O3 which were impregnated with platinum in terms of catalytic activity for propane dehydrogenation and physicochemical properties. 1.5 wt% Pt, 0-10 wt% Cu catalyst supported on θ-Al2O3 or γ-Al2O3 was prepared by incipient wetness co-impregnation. Enhanced Pt dispersion by increasing Cu contents in γ-Al2O3 supported catalyst was confirmed via XRD and XPS. Pt and CuO was separated in Pt-Cu/θ-Al2O3, but Pt-Cu alloy was identified after reduction treatment. Also, adding Cu in Pt/Al2O3 makes catalyst’s acidity lower and this property led to increased propylene yield in propane dehydrogenation. However, Pt3Cu was not good for yield of PDH, which was confirmed in Pt-10Cu/θ-Al2O3 through XRD.  相似文献   

3.
A series of phosphotungstic acid (HPW)/SiO2 materials with hierarchical meso/macroporous structure were synthesized by evaporation-induced self-assembly method (EISA), using nonionic surfactant (P123) and polystyrene (PS) spheres as templates. SEM images displayed uniform macropores with an average pore size of 210 nm. TEM, small-angle XRD and N2 adsorption–desorption isotherms confirmed the existence of the ordered mesoporous structures, embedded in the wall of macropores. The wild-angle XRD and FT-IR spectra proved Keggin-type HPW dispersed homogeneously in the silica framework. With the amount of added PS spheres, the density of the macropores increased, the hierarchically ordered porous HPW/SiO2 possessed two-dimensional (2D) hexagonal (p6mm) mesostructures and uniform periodic macropores. The ODS catalytic activity of these samples were tested, the result showed that the meso/macroporous HPW/SiO2 catalyst with proper PS beads usage displayed much higher catalytic activity than other catalysts. In addition, the reusability of the meso/macroporous HPW/SiO2 catalyst was investigated, the activity of catalyst has not obviously decreased even after eight times.  相似文献   

4.
In this study, we developed an original approach for preparing cellulose-coated magnetite nanoparticles (NPs). Two novel Schiff bases (PDA-g-DAC) and [Bz-(PDA-g-DAC)] were synthesized via condensation reactions of periodate oxidized micro-crystalline cellulose (DAC) with o-phenylene diamine (PDA) to obtain its azomethine derivative with 85% yield. Subsequently, the functionalization of (PDA-g-DAC) with benzil (Bz) yields the tetraaza macrocycle [Bz-(PDA-g-DAC)]. The physicochemical characterization of the condensation products was performed using 13CNMR, FTIR, ATG, DSC, and X-ray diffraction techniques. Magnetic nanomaterial-based Schiff base cellulose was successfully prepared using in situ chemical co-precipitation of coordinated ferric and ferrous ions in cellulose Schiff base matrix under optimized conditions, and then, its magnetic properties were characterized. The results demonstrated that the Fe3O4 NPs coated with [Bz-(PDA-g-DAC)] were homogeneously coated in the matrix under ultrasonic irradiation with the saturation magnetization of 69.50 emu g?1. In addition, XRD line broadening analysis showed that the average particle size of the NPs was 37.3 nm. Furthermore, FTIR spectra demonstrated that [Bz-(PDA-g-DAC)] concavity was anchored to magnetite Fe3O4 NPs through azomethine groups. Vibrating sample magnetometry (VSM) of [Bz-(PDA-g-DAC)@Fe3O4] magnetic nanocomposite samples showed the typical behavior of ferromagnetism. This study provided a green and facile method to inhibit magnetic nanoparticle aggregation. Activity results revealed that the prepared [Bz-(PDA-g-DAC)@Fe3O4] catalyst shows the maximum activity for degradation of Acid Yellow 17 (AY17) compared to other prepared catalysts. After degradation reaction, the [Bz-(PDA-g-DAC)@Fe3O4] catalyst was recovered from the reaction mixture via an external magnet and used for further five consecutive cycles with excellent catalytic activity, successively, which was comparable to the fresh catalyst. The catalyst degradation efficiency and its easy separation exhibited that [Bz-(PDA-g-DAC)@Fe3O4] catalyst is a promising material for the removal of AY17 from aqueous solutions in green chemistry perspectives.  相似文献   

5.
Vanadium oxide supported on zirconia modified with WO3 was prepared by adding Zr(OH)4 powder into a mixed aqueous solution of ammonium metavanadate and ammonium metatungstate followed by drying and calcining at high temperatures. The characterization of prepared catalysts was performed by using FTIR, Raman, and XRD. In the case of calcination temperature at 773 K, for samples containing low loading V2O5 below 18 wt%, vanadium oxide was in a highly dispersed state, while for samples containing high loading V2O5 equal to or above 18 wt%, vanadium oxide was well crystallized due to the high V2O5 loading on the surface of ZrO2. The ZrV2O7 compound was formed through the reaction of V2O5 and ZrO2 at 873 K, and the compound decomposed into V2O5 and ZrO2 at 1,073 K, these results were confirmed by FTIR and XRD. Catalytic tests for 2-propanol dehydration and cumene dealkylation have shown that the addition of WO3 to V2O5/ZrO2 enhanced both catalytic activity and acidity of V2O5-WO3/ZrO2 catalysts. The variations in catalytic activities for both reactions are roughly correlated with the changes of acidity.  相似文献   

6.
Oxidative dehydrogenation of n-butene to 1,3-butadiene over sulfated ZnFe2O4 catalyst was carried out in a continuous flow fixed-bed reactor. The effect of sulfation on the catalytic performance of ZnFe2O4 was investigated. Sulfated ZnFe2O4 catalyst showed a better catalytic performance than ZnFe2O4 catalyst in the oxidative dehydrogenation of n-butene. Acid–base property of sulfated ZnFe2O4 catalyst was measured by TPD experiment, with an aim of correlating the catalytic performance with the surface acid–base property of the catalyst. It was revealed that the catalytic performance of sulfated ZnFe2O4 catalyst was closely related to the surface weak-acid density of the catalyst. The enhanced acidity of sulfated ZnFe2O4 catalyst was responsible for its high catalytic performance in the oxidative dehydrogenation of n-butene. Thus, sulfation served as an efficient method for improving catalytic performance of ZnFe2O4 in the oxidative dehydrogenation of n-butene.  相似文献   

7.
Spherical carbon (SC) with a diameter of ca. 9 μm was synthesized by a hydrothermal method using sucrose as a carbon precursor. The spherical carbon was then modified to have a positive charge, and thus, to provide a site for the immobilization of H5PMo10V2O40 (PMo10V2) catalyst. The PMo10V2 catalyst was immobilized on the surface-modified spherical carbon by taking advantage of the overall negative charge of [PMo10V2O40]5−. The PMo10V2 catalyst immobilized on the spherical carbon (PMo10V2/SC) was applied to the vapor-phase 2-propanol conversion reaction. In the catalytic reaction, the PMo10V2/SC catalyst showed a higher 2-propanol conversion than the unsupported PMo10V2 catalyst. Furthermore, the PMo10V2/SC catalyst showed enhanced oxidation catalytic activity (formation of acetone) and the suppressed acid catalytic activity (formation of propylene and isopropyl ether) compared to the unsupported PMo10V2 catalyst. The enhanced oxidation activity of PMo10V2/SC catalyst was due to the fine dispersion of [PMo10V2O40]5− on the spherical carbon formed via chemical immobilization.  相似文献   

8.
It is difficult to research on the surface structure of amorphous phase in fly ash during leaching reaction due to crystalline phase and complex structure. In the present work, in order to reveal the effects of leaching reaction on the surface structure of amorphous phase in fly ash, the modelling CaO-Fe2O3-Al2O3-SiO2 glass was prepared by the traditional melting methods. The leaching reaction of CaO-Fe2O3-Al2O3-SiO2 glass with 7.5 M KOH was investigated by spectroscopy, spectrophotometer and wet chemical method. The results show that the content of Q 1, Q 2, Q 3 and Q 4 of glass without corrosion was 4.21, 9.51, 23.03 and 52.55%, respectively, which shows that the network polymerization of glass is compact. The leaching reaction of glass can be described by the following equation: dS/dt = k/(r + S 0). Leaching in KOH for various times induces the content of Q 4 and Q 1 to be decreased, and Q 2 and Q 3 increased, resulted in the depolymerization of network and the surface glass dissolved in alkaline solution to form a gel phase. In stage one of leaching reaction, the rate of iron ion leached from glass surface was slow, which resulted in the small slope of straight-line relationship of leaching curve. In the following stage, the leaching rate of iron ion increased with the prolongation of time.  相似文献   

9.
The crystal structure of Pb6O[(Si6Al2)O20)] is investigated using X-ray diffraction. The compound has tetragonal symmetry, space group I4/mmm, a = 11.7162(10) Å, c = 8.0435(12) Å, and V = 1104.13(2) Å3. The structure is refined to R 1 = 0.036 for 562 unique reflections with [F 0] ≥ 4σF. The structure contains two symmetrically independent positions of the Pb2+ cations coordinated by five O atoms (Pb2+-O2? = 2.34–2.68 Å). The TO4 tetrahedra (T = Si, Al) form tubular [(Si6Al2)O20] chains extended along the c axis. The O4 oxygen atom is not bonded to the Si and Al atoms and is octahedrally coordinated by six Pb atoms with the formation of an oxo-centered OPb6 octahedron. The assumption is made that, in some of lead silicate and aluminosilicate glasses, a number of oxygen atoms are located outside the tetrahedral structure and represent segregation centers of the Pb2+ cations due to the formation of oxo-centered complexes.  相似文献   

10.
A new compound, CdPb2O2Cl2, is synthesized by the method of solid-phase reactions. The compound has monoclinic symmetry, space group C2/m, a = 12.392(8) Å, b = 3.8040(14) Å, c = 7.658(5) Å, β = 122.64(5)°, and V = 304.0(3) Å3. The structure contains one symmetrically independent position of the Pb2+ cation coordinated by three O2? anions (Pb2+-O2? = 2.29–2.34 Å) and five Cl? anions (Pb2+-Cl? = 3.35–3.57 Å). The Cd2+ cation has a symmetric coordination with the formation of two bonds Cd-O = 2.15 Å and four bonds Cd-Cl = 2.73 Å. The oxygen atom is tetrahedrally coordinated by three Pb2+ cations and one Cd2+ cation, which leads to the formation of oxo-centered heterometallic OPb3Cd tetrahedra. The tetrahedra are linked together into chains through common Pb atoms and into layered complexes due to sharing of the equatorial Cd atoms. The chlorine atoms are located above the cavities of the oxo-centered layer.  相似文献   

11.
A cathode material for lithium-ion batteries–LiNi1/3Co1/3Mn1/3O2–was prepared by solution combustion synthesis and characterized by XRD, SEM, and galvanostatic charge/discharge cycling. The sample calcined at 950°C for 10 h showed best charge/discharge performance. An initial discharge capacity (C) of 150.5 mA h g–1 retained 95.7% of its value after 75 charge/discharge cycles at Ic = 14 mA g–1 (0.2C rate), Id = 70 mA g–1 (0.5C rate).  相似文献   

12.
A series of V2O5-TiO2 aerogel catalysts were prepared by the sol-gel method with subsequent supercritical drying with CO2. The main variables in the sol-gel method were the amounts of V2O5 and when the vanadium precursor was introduced. V2O5-TiO2 xerogel and V2O5/TiO2 (P-25) were also prepared for comparison. The V2O5-TiO2 aerogel catalysts showed much higher surface areas and total pore volumes than V2O5-TiO2 xerogel and impregnated V2O5/TiO2 (P-25) catalysts. The catalysts were characterized by N2 physisorption, X-ray diffraction (XRD), FT-Raman spectroscopy, temperature-programmed reduction with H2 (H2-TPR), and temperature-programmed desorption of ammonia (NH3-TPD). The selective catalytic reduction of NOx with ammonia in the presence of excess O2 was studied over these catalysts. Among various V2O5-TiO2 catalysts, V2O5 supported on aerogel TiO2 showed a wide temperature window exhibiting high NOx conversions. This superior catalytic activity is closely related to the large amounts of strong acidic sites as well as the surface vanadium species with characteristics such as easy reducibility and monomeric and polymeric vanadia surface species. This work was presented at the 7 th Korea-China Workshop on Clean Energy Technology held at Taiyuan, Shanxi, China, June 26–28, 2008.  相似文献   

13.
Novel highly active visible-light photocatalysts in the form of zinc bismuth oxide (ZnBi2O4) and graphite hybrid composites were prepared by coupling via a co-precipitation method followed by calcination at 450 °C. The as-prepared ZnBi2O4-graphite hybrid composites were tested for the degradation of rhodamine B (RhB) solutions under visible-light irradiation. The existence of strong electronic coupling between the two components within the ZnBi2O4-graphite heterostructure suppressed the photogenerated recombination of electrons and holes to a remarkable extent. The prepared composite exhibited excellent photocatalytic activity, leading to more than 93% of RhB degradation at an initial concentration of 50mg·L-1 with 1.0 g catalyst per liter in 150min. The excellent visible-light photocatalytic mineralization of ZnBi2O4-1.0graphite in comparison with pristine ZnBi2O4 could be attributed to synergetic effects, charge transfer between ZnBi2O4 and graphite, and the separation efficiency of the photogenerated electrons and holes. The photo-induced h+ and the superoxide anion were the major active species responsible for the photodegradation process. The results demonstrate the feasibility of ZnBi2O4-1.0graphite as a potential heterogeneous photocatalyst for environmental remediation.  相似文献   

14.
This study considers the feasibility of uptake of cephalexin, an emerging contaminant, from aqueous solutions by using green local montmorillonite (GLM), montmorillonite coated with ZnO (ZnO/GLM) and montmorillonite coated with TiO2 (TiO2/GLM) in the presence of H2O2. Batch adsorption experiments were carried out as a function of pH, initial concentration of the cephalexin, adsorbent dosage, contact time, and temperature. Finally, the adsorbents were characterized by XRD, SEM and FTIR analyses. XRD patterns showed dramatic changes in the adsorbents after loading with the nanoparticles, confirming successful placing of the nanoparticles onto GLM. The GLM mineral surface after nanoparticle loading appears to be fully exposed and more porous with irregular shapes in particles diameters of 1-50 microns. FTIR analyses also confirmed dramatic changes in surface functional groups after modification with these nanoparticles. The results showed that the removal efficiency of cephalexin was better at lower pH values. Totally, the removal efficiency increased with increase in adsorbent dosage and contact time and decreased with concentration and temperature increase. The thermodynamics values of ΔG o and ΔH o revealed that the adsorption process was spontaneous and exothermic. In isotherm study, the maximum adsorption capacities (qm) were obtained to be 7.82, 17.09 and 49.26 mg/g for GLM, ZnO/GLM and TiO2/GLM, respectively. Temkin constant (B T ) showed that adsorption of cephalexin from solution was exothermic for all three adsorbents.  相似文献   

15.
The density d at a temperature of 25°C is measured by the hydrostatic weighing method, the Vickers microhardness H V is determined, and the fluctuation free volume fraction f g is calculated for glasses in the SrO-B2O3-SiO2 system with a constant strontium oxide content in the range from 35 to 45 mol %. It is demonstrated that the quantities H V and f g decrease and the density d increases with an increase in the SrO content.  相似文献   

16.
The ramsdellite-type phases crystallizing in the Li2O-Fe2O3-TiO2 system in the course of synthesis in gaseous media at different oxygen partial pressures are studied. Solid solutions based on the ramsdellite structure with the composition Li2Ti3?xFe x O7 ? δ (0 ≤ x ≤ 0.7) are prepared in an oxidizing medium (PO2 = 1 atm) for the first time. Analysis of the results obtained by electron paramagnetic resonance and Mossbauer spectroscopy revealed that, in these solid solutions, all iron ions are in the oxidation state Fe+3.  相似文献   

17.
TiO2-Al2O3 mixed oxides with different compositions ranging from 40wt-% to 95wt-% of TiO2 were prepared by sol-gel method and impregnated with different amounts of VO x . Supports and catalysts were characterized by X-ray diffraction (XRD), physisorption, temperature preprogrammed reduction (H2-TPR), and ammonia temperature programmed desorption (NH3-TPD). TiO2 content in the support had obvious effect on the crystal structure, texture characteristic, acid property, and catalytic activity in dehydrogenation of ethylbenzene (EB) with carbon dioxide. The highest catalytic activity was acquired when the TiO2 content was 50 wt-%.  相似文献   

18.
A new green chemical route was designed in this paper for the synthesis of high-silica EU-1 molecular sieve in TEAOH–SiO2–Al2O3–HMBr2–H2O system in which tetraethylammonium hydroxide (TEAOH) substituted for sodium hydroxide (NaOH) as an alkali source. The physicochemical properties of the synthesized samples characterized by such means as X-ray powder diffraction (XRD), electrophoresis apparatus, precise pH meter, scanning electron microscope, Fourier infrared spectrometer (FT-IR), thermo gravimetric analyzer (TG) and temperature programmed desorption (NH3-TPD). The research results showed that the SiO2/Al2O3 ratio of EU-1 molecular sieve could reach 706 with TEAOH as an alkali source. The SiO2/Al2O3 ratio of the product was improved greatly to 1046 with the template agent increasing. The new synthetic route has also significantly expanded the synthetic phase region. The absolute value of zeta potential of the TEAOH sol system was obviously higher than that of the NaOH sol system, indicating the thermodynamic stability of the former sol system was higher and better for the synthesis of pure high-silica EU-1 molecular sieve. The FT-IR spectra and TG/DTG diagrams of products indicated that TEA+ occluded in the final products could balance electronegative framework. The amount of strong, weak and the total acidity reduced with the increase of SiO2/Al2O3 ratio. The catalytic results of methanol-to-hydrocarbon demonstrated that the molecular sieve prepared by the new method has better catalytic performance.  相似文献   

19.
Anhydrous ammonium pentaborate NH4B5O8 has been synthesized by thermal dehydration of larderellite NH4[B5O7(OH)2] · H2O at a temperature of 290°C for 7 h. The crystal structure has been determined from the X-ray powder diffraction data: a = 7.58667(5) Å, b = 12.00354(8) Å, c = 14.71199(8) Å, R p = 6.23, R wp = 7.98, R B = 12.7, R F = 8.95, and β-KB5O8 structure type. The double interpenetrating framework is formed by pentaborate groups, each consisting of a boron-oxygen tetrahedron and four triangles, in which all oxygen atoms are bridging. The thermal behavior of the NH4B5O8 compound has been investigated using thermal X-ray diffraction. As for other pentaborates of this type, the thermal expansion of the NH4B5O8 compound is anisotropic and reaches a maximum along the a axis. The thermal expansion coefficients are as follows: α a = 39 × 10?6, α b = 6 × 10?6, α c = 20 × 10?6, and α V = 65 × 10?6 °C?1.  相似文献   

20.
A new compound of (Rb,K)2Cu3(P2O7)2 is obtained by high-temperature reactions from a mixture of RbNO3, KNO3, Cu(NO3)2, and (NH4)4P2O7. The crystal structure was solved by direct methods and refined to R 1 = 0.056 for 5022 independent reflections. The compound belongs to a rhombic crystal system, P212121, Z = 8, a = 9.9410(7) Å, b = 13.4754(6) Å, c = 18.6353 (3) Å, and R = 0.056. The basis of the structure is a complex copper-phosphate skeleton of the composition of [Cu3(P2O7)2]2–, which can be regarded as consisting of two types of heteropolyhedral layers parallel to the (001) plane. The layers are alternated with each other, forming a frame, in the cavities of which the positions of alkali cations are located, statistically populated with K+ and Rb+ ions. Based on the refined populations of the positions of alkali cations, an exact chemical formula of the compound can be written as Rb1.28K0.72Cu3(P2O7)2. The compound is the most complex among those known to this day of the composition of A2 IB3 II(P2O7)2 (A = Li, Na, K, Rb, or Cs; B = Ni, Cu, or Zn).  相似文献   

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