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1.
La xSr 2−xMnO 4 (0 ≤ x ≤ 0.8) oxides were synthesized and single-phase K 2NiF 4-type oxides were obtained in the range of 0.1 ≤ x < 0.5. The catalytic activity of La xSr 2−xMnO 4 for NO–CO reaction increased with increasing x in the range of solubility limit of La. La 0.5Sr 1.5MnO 4 showed the highest activity among La xSr 2−xMnO 4 prepared in this study, but its activity was inferior to perovskite-type La 0.5Sr 0.5MnO 3. Among the Pd-loaded catalysts, however, Pd/La 0.8Sr 1.2MnO 4 showed the higher activity and the selectivity to N 2 than Pd/La 0.5Sr 0.5MnO 3 and Pd/γ-Al 2O 3. The excellent catalytic performance of Pd/La 0.2Sr 1.2MnO 4 could be ascribable to the formation of SrPd 3O 4 which was detected by XRD in the catalyst but not in the other two catalysts. 相似文献
2.
Ultrafine lithium ion conducting La 2/3−xLi 3xTiO 3 ( x = 0.11, LLT) powder was synthesized by a simple polymerizable complex method based on the Pechini-type process. The formation mechanism, homogeneity and microstructure of the samples were investigated by thermal analysis (TG/DTA), X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). XRD analysis indicated the formation of pure perovskite-type phase. The powder synthesized at a temperature as low as 900 °C in a much shorter time than solid-state reaction method was well crystallized. The lithium ion conductivity of the LLT ceramics sintered at 1200 °C was found to be 9 × 10 −4 S/cm at room temperature. 相似文献
3.
Ceramics with a composition close to BaZn 2Ti 4O 11 were synthesized according to various substitutional mechanisms in order to verify an existence of a homogeneity range in the vicinity of this composition. Structural and microstructural investigations showed that the crystal structure of BaZn 2Ti 4O 11 was formed in the homogeneity range corresponding to the formula BaZn 2 − xTi 4O 11 − x (0 < x < 0.1). Densely sintered BaZn 2 − xTi 4O 11 − x (0 < x < 0.1) ceramics exhibited a dielectric constant around 30, τf = −30 ppm/K and high Q × f values, which increased from 68,000 GHz at x = 0 to 83,000 GHz at x = 0.05. Structurally, the deficiency of Zn in BaZn 2 − xTi 4O 11 − x (0 < x < 0.1) resulted in a slight decrease in the unit-cell volume. The influence of secondary phases in the BaZn 2Ti 4O 11-based materials on the microwave dielectric properties was also investigated. A presence of small amounts of ZnO, BaTiO 3, hollandite-type solid solutions (Ba xZn xTi 8 − xO 16) and BaTi 4O 9 caused a decrease in Q × f values. 相似文献
4.
The structure evolution, and microwave dielectric properties of Nd (2−x)/3Li xTiO 3 ceramics (0 ≤ x ≤ 0.5) were investigated in this paper. X-ray diffraction (XRD) and scanning electron microscopy (SEM) results show that samples with x = 0.2–0.4 exhibit single phase. Multi-phases of Nd 2Ti 2O 7, Nd 2/3TiO 3 and Nd 2Ti 4O 11 were observed when x = 0 and 0.1. The concentration and ordering degree of A-site decrease with the increase of x value. The dielectric constant increases up to x = 0.2 and then decreases with the further increase of x value. The Qf value decreases with the increase of x value. The temperature coefficient of resonant frequency exhibits negative value and the absolute value decreases greatly with the decrease of x value. 相似文献
5.
Layered Li[Ni (1−x)/3Mn (1−x)/3Co (1−x)/3Cr x]O 2 materials with x = 0, 0.01, 0.02, 0.03, 0.05 are prepared by a solid-state pyrolysis method. The oxide compounds were calcined with various Cr-doped contents, which result in greater difference in morphological (shape, particle size and specific surface area) and the electrochemical (first charge profile, reversible capacity and rate capability) differences. The Li[Ni (1−x)/3Mn (1−x)/3Co (1−x)/3Cr x]O 2 powders were characterized by means of X-ray diffraction (XRD), charge/discharge cycling, cyclic voltammetry, and SEM. XRD experiment revealed that the Li[Ni (1−x)/3Mn (1−x)/3Co (1−x)/3Cr x]O 2 ( x = 0, 0.01, 0.02, 0.03, 0.05) were crystallized to well layered -NaFeO 2 structure. The first specific discharge capacity and coulombic efficiency of the electrode of Cr-doped materials were higher than that of pristine material. When x = 0.02, the sample showed the highest first discharge capacity of 241.9 mAh g −1 at a current density of 30 mA g −1 in the voltage range 2.3–4.6 V, and the Cr-doped samples exhibited higher discharge capacity and better cycleability under medium and high current densities at room temperature. 相似文献
6.
The sintering properties of La 1−xSr xFeO 3−δ ( x = 0.1, 0.25) mixed conductors have been investigated with particular emphasis on the effect of secondary phases due to cation non-stoichiometry (±5 mol% La excess and deficiency). Secondary phases, located at grain boundaries in cation non-stoichiometric materials, increased the sintering temperature compared to single-phase materials. Extensive swelling in final stage of sintering was observed in all materials, which resulted in micro-porous materials. The swelling was most pronounced in the phase pure and two-phase materials due to La-deficiency, while refractory secondary phases in La-excess materials inhibited both sintering, grain growth and swelling. In La-deficient materials, formation of molten secondary phases resulted in rapid swelling due to viscous flow. The present findings demonstrated the importance of controlling sintering temperature and time, as well as careful control of the cation stoichiometry of La 1−xSr xFeO 3−δ in order to achieve fully dense and homogenous La 1−xSr xFeO 3−δ ceramics. 相似文献
7.
Electrical resistivity and Seebeck ( S) measurements were performed on (La 1−xSr x)MnO 3 (0.02 x0.50) and (La 1−xSr x)CoO 3 (0 x0.15) in air up to 1073 K. (La 1−xSr x)MnO 3 ( x0.35) showed a metal-to-semiconductor transition; the transition temperature almost linearly increased from 250 to 390 K with increasing Sr content. The semiconductor phase above the transition temperature showed negative values of S. (La 1−xSr x)CoO 3 (0 x0.10) showed a semiconductor-to-metal transition at 500 K. Dominant carriers were holes for the samples of x0.02 above room temperature. LaCoO 3 showed large negative values of S below ca. 400 K, indicative of the electron conduction in the semiconductor phase. 相似文献
8.
Perovskites of different La 1−xSr xAl 1−y−y′Fe yMg y′O 3−δ compositions ( x=0, 0.1, 0.15, 0.2 and y=0.1, 0.3, 0.5, 0.8) were prepared from a reactive precursor slurry of hydrated oxides. Each sample was aged between 16 and 26 h up to 1473 K. Activity in methane combustion (1%/air) was determined in a plug-flow reactor, with 1 g catalyst and 24 l/h flowrate. Gradual decrease in activity due to thermal aging was observed, the degree of activity loss being composition dependent. Nevertheless, activity of samples aged at 1370 K was nearly independent of composition. The best thermal stability showed LaAl 0.65Fe 0.15Mg 0.2O 3 perovskite. None of the magnesium substituted perovskites performed better than a La 0.85Sr 0.15Al 0.87Fe 0.13O 3 reference sample. 相似文献
9.
The activities of perovskites depend on compositions and preparation methods. Various perovskites, La 1−xM xMnO 3 (M=Ag, Sr, Ce, La), have been prepared by two different methods (co-precipitation and spray decomposition). The new preparation method, spray decomposition, produced perovskites of a high surface area of over 10 m 2/g. The catalytic activities for CH 4 and CO oxidation have been studied on a series of catalysts, La 1−xM xMnO 3. The perovskite-type oxide, La 0.7Ag 0.3MnO 3, shows the highest catalytic activity: the complete conversion of CO and CH 4 at 370 and 825 K, respectively. 相似文献
10.
Catalytic methane combustion and CO oxidation were investigated over AFeO 3 (A=La, Nd, Sm) and LaFe 1−xMg xO 3 ( x=0.1, 0.2, 0.3, 0.4, 0.5) perovskites prepared by citrate method and calcined at 1073 K. The catalysts were characterized by X-ray diffraction (XRD). Redox properties and the content of Fe 4+ were derived from temperature programmed reduction (TPR). Specific surface areas (SA) of perovskites were in 2.3–9.7 m 2 g −1 range. XRD analysis showed that LaFeO 3, NdFeO 3, SmFeO 3 and LaFe 1−xMg xO 3 ( x·0.3) are single phase perovskite-type oxides. Traces of La 2O 3, in addition to the perovskite phase, were detected in the LaFe 1−xMg xO 3 catalysts with x=0.4 and 0.5. TPR gave evidence of the presence in AFeO 3 of a very small fraction of Fe 4+ which reduces to Fe 3+. The fraction of Fe 4+ in the LaFe 1−xMg xO 3 samples increased with increasing magnesium content up to x=0.2, then it remained nearly constant. Catalytic activity tests showed that all samples gave methane and CO complete conversion with 100% selectivity to CO 2 below 973 and 773 K, respectively. For the AFeO 3 materials the order of activity towards methane combustion is La>Nd>Sm, whereas the activity, per unit SA, of the LaFe 1−xMg xO 3 catalysts decreases with the amount of Mg at least for the catalysts showing a single perovskite phase ( x=0.3). Concerning the CO oxidation, the order of activity for the AFeO 3 materials is Nd>La>Sm, while the activity (per unit SA) of the LaFe 1−xMg xO 3 catalysts decreases at high magnesium content. 相似文献
11.
(Mg 1−xZn x) 2SiO 4 ceramics were prepared and characterized. The densification temperatures of the present ceramics are much lower than those for Mg 2SiO 4 and Zn 2SiO 4 end-members. Small solid solution limits of Zn in Mg 2SiO 4 and Mg in Zn 2SiO 4 are observed, and the bi-phase structure is confirmed in (Mg 1−xZn x) 2SiO 4 ceramics with x = 0.1–0.9. Even though, it is clear that the Qf value of Zn 2SiO 4 ceramics can be significantly improved together with a suppressed temperature coefficient of resonant frequency τf by substituting Mg for Zn. (Mg 0.4Zn 0.6) 2SiO 4 ceramics indicate a good combination of microwave dielectric characteristics: r = 6.6 Qf = 95,650 GHz, and τf = −60 ppm/°C. 相似文献
12.
A series of the Ce 1−xCu xO 2−x/Al 2O 3/FeCrAl catalysts ( x = 0–1) were prepared. The structure of the catalysts was characterized using XRD, SEM and H 2-TPR. The catalytic activity of the catalysts for the combustion of methane was evaluated. The results indicated that in the Ce 1−xCu xO 2−x/Al 2O 3/FeCrAl catalysts the surface phase structure were the Ce 1−xCu xO 2−x solid solution, -Al 2O 3 and γ-Al 2O 3. The surface particle shape and size were different with the variety of the molar ratio of Ce to Cu in the Ce 1−xCu xO 2−x solid solution. The Cu component of the Ce 1−xCu xO 2−x/Al 2O 3/FeCrAl catalysts played an important role to the catalytic activity for the methane combustion. There were the stronger interaction among the Ce 1−xCu xO 2−x solid solution and the Al 2O 3 washcoats and the FeCrAl support. 相似文献
13.
Ten weight percent BBZS (Bi 2O 3, B 2O 3, ZnO and SiO 2) glass was added to x(Ba 4Nd 9.333Ti 18O 54) − (1 − x)(BaLa 4Ti 4O 15) (BNLT, 0 ≤ x ≤ 1) composite dielectric ceramics to lower their sintering temperature whilst retaining microwave properties useful for low temperature co-fired ceramic and antenna core technology. With the addition of 10 wt% BBZS glass, dense BNLT composite ceramics were produced at temperatures between 950 and 1140 °C, depending on composition ( x), an average reduction of sintering temperature by 350 °C. X-ray diffraction, scanning and transmission electron microscopy and Raman spectroscopy studies revealed that there was limited inter-reaction between BLT/BNT and the BBZS glass. Microwave property measurement showed that the addition of BBZS glass to BNLT ceramics had a negligible effect on r and τf, although deterioration in the measured quality factor ( Qf) was observed. The optimised composition ( xBNT − (1 − x)BLT)/0.1BBZS ( x = 0.75) had r 61, τf 38 ppm/°C and Qf 2305 GHz. 相似文献
14.
Nanometer perovskite-type oxides La 1−xSr xMO 3−δ (M = Co, Mn; x = 0, 0.4) have been prepared using the citric acid complexing-hydrothermal-coupled method and characterized by means of techniques, such as X-ray diffraction (XRD), BET, high-resolution scanning electron microscopy (HRSEM), X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption (TPD), and temperature-programmed reduction (TPR). The catalytic performance of these nanoperovskites in the combustion of ethylacetate (EA) has also been evaluated. The XRD results indicate that all the samples possessed single-phase rhombohedral crystal structures. The surface areas of these nanomaterials ranged from 20 to 33 m 2 g −1, the achievement of such high surface areas are due to the uniform morphology with the typical particle size of 40–80 nm (as can be clearly seen in their HRSEM images) that were derived with the citric acid complexing-hydrothermally coupled strategy. The XPS results demonstrate the presence of Mn 4+ and Mn 3+ in La 1−xSr xMnO 3−δ and Co 3+ and Co 2+ in La 1−xSr xCoO 3−δ, Sr substitution induced the rises in Mn 4+ and Co 3+ concentrations; adsorbed oxygen species (O −, O 2−, or O 22−) were detected on the catalyst surfaces. The O 2-TPD profiles indicate that Sr doping increased desorption of the adsorbed oxygen and lattice oxygen species at low temperatures. The H 2-TPR results reveal that the nanoperovskite catalysts could be reduced at much lower temperatures (<240 °C) after Sr doping. It is observed that under the conditions of EA concentration = 1000 ppm, EA/oxygen molar ratio = 1/400, and space velocity = 20,000 h −1, the catalytic activity (as reflected by the temperature ( T100%) for EA complete conversion) increased in the order of LaCoO 2.91 ( T100% = 230 °C) ≈ LaMnO 3.12 ( T100% = 235 °C) < La 0.6Sr 0.4MnO 3.02 ( T100% = 190 °C) < La 0.6Sr 0.4CoO 2.78 ( T100% = 175 °C); furthermore, there were no formation of partially oxidized by-products over these catalysts. Based on the above results, we conclude that the excellent catalytic performance is associated with the high surface areas, good redox properties (derived from higher Mn 4+/Mn 3+ and Co 3+/Co 2+ ratios), and rich lattice defects of the nanostructured La 1−xSr xMO 3−δ materials. 相似文献
15.
Nanoparticles of Ce xZr 1−xO 2 ( x = 0.75, 0.62) were prepared by the oxidation-coprecipitation method using H 2O 2 as an oxidant, and characterized by N 2 adsorption, XRD and H 2-TPR. Ce xZr 1−xO 2 prepared had single fluorite cubic structure, good thermal stability and reduction property. With the increasing of Ce/Zr ratio, the surface area of Ce xZr 1−xO 2 increased, but thermal stability of Ce xZr 1−xO 2 decreased. The surface area of Ce 0.62Zr 0.38O 2 was 41.2 m 2/g after calcination in air at 900 °C for 6 h. TPR results showed the formation of solid solution promoted the reduction of CeO 2, and the reduction properties of Ce xZr 1−xO 2 were enhanced by the cycle of TPR-reoxidation. The Pd-only three-way catalysts (TWC) were prepared by the impregnation method, in which Ce 0.75Zr 0.25O 2 was used as the active washcoat and Pd loading was 0.7 g/L. In the test of Air/Fuel, the conversion of C 3H 8 was close to 100% and NO was completely converted at λ < 1.025. The high conversion of C 3H 8 was induced by the steam reform and dissociation adsorption reaction of C 3H 8. Pd-only catalyst using Ce 0.75Zr 0.25O 2 as active washcoat showed high light off activity, the reaction temperatures ( T50) of 50% conversion of CO, C 3H 8 and NO were 180, 200 and 205 °C, respectively. However, the conversions of C 3H 8 and NO showed oscillation with continuously increasing the reaction temperature. The presence of La 2O 3 in washcoat decreased the light off activity and suppressed the oscillation of C 3H 8 and NO conversion. After being aged at 900 °C for 4 h, the operation windows of catalysts shifted slightly to rich burn. The presence of La 2O 3 in active washcoat can enhance the thermal stability of catalyst significantly. 相似文献
16.
Catalytic combustion of methane has been investigated over AMnO 3 (A = La, Nd, Sm) and Sm 1−xSr xMnO 3 ( x = 0.1, 0.3, 0.5) perovskites prepared by citrate method. The catalysts were characterized by chemical analysis, XRD and TPR techniques. Catalytic activity measurements were carried out with a fixed bed reactor at T = 623–1023 K, space velocity = 40 000 N cm 3 g −1 h −1, CH 4 concentration = 0.4% v/v, O 2 concentration = 10% v/v. Specific surface areas of perovskites were in the range 13–20 m2 g−1. XRD analysis showed that LaMnO3, NdMnO3, SmMnO3 and Sm1−xSrxMnO3 (x = 0.1) are single phase perovskite type oxides. Traces of Sm2O3 besides the perovskite phase were detected in the Sm1−xSrxMnO3 catalysts for x = 0.3, 0.5. Chemical analysis gave evidence of the presence of a significant fraction of Mn(IV) in AMnO3. The fraction of Mn(IV) in the Sm1−xSrxMnO3 samples increased with x. TPR measurements on AMnO3 showed that the perovskites were reduced in two steps at low and high temperature, related to Mn(IV) → Mn(III) and Mn(III) → Mn(II) reductions, respectively. The onset temperatures were in the order LaMnO3 > NdMnO3 > SmMnO3. In Sm1−xSrxMnO3 the Sr substitution for Sm caused the formation of Mn(IV) easily reducible to Mn(II) even at low temperature. Catalytic activity tests showed that all samples gave methane complete conversion with 100% selectivity to CO2 below 1023 K. The activation energies of the AMnO3 perovskites varied in the same order as the onset temperatures in TPR experiments suggesting that the catalytic activity is affected by the reducibility of manganese. Sr substitution for Sm in SmMnO3 perovskites resulted in a reduction of activity with respect to the unsubstituted perovskite. This behaviour was related to the reduction of Mn(IV) to Mn(II), occurring under reaction conditions, hindering the redox mechanism. 相似文献
17.
Perovskite type La 1 − xSr xMnO 3 ( x = 0–0.5) oxides were prepared by the amorphous citrate process, characterised by X-ray diffraction, oxygen desorption, temperature-programmed reduction, infrared and X-ray photoelectron spectroscopic techniques, and tested for methane combustion within the 473–1073 K temperature range. Since catalyst activity was found to depend strongly on BET areas and to a lesser extent, on the degree of substitution ( x), intrinsic activities were computed for La 1 − xSr xMnO 3 catalyst series. Among the compositions investigated, the degree of substitution x = 0.2 showed the highest intrinsic activity within the temperatures explored. Characterisation techniques made possible to correlate catalytic performance with the structural characteristics of the oxides. The stability of Mn 4+ is probably the most important parameter, but excess of oxygen and atomic surface composition should also be taken into account. 相似文献
18.
The effect of introduction of alkalies (Me = Li, K, Cs) into SrTiO 3 on the physico-chemical properties of resulted materials and their catalytic activity in soot combustion was studied. Two groups of SrTiO 3 based perovskites were prepared: substituted in A-position of the structure (Sr 1 − xMe xTiO 3, x = 0.05–0.2) and impregnated with the same amount of alkali metals. Prepared materials exhibit low specific surface area and perovskite structure, only these ones impregnated with the highest amount of Cs (K) show weak XRD signals of Me 2O. TPD-O 2 experiments show bimodal profiles of O 2 desorption curves with maximums corresponding to individual step of alkali nitrates thermal decomposition. It is supposed that second peak of O 2 desorption from impregnated SrTiO 3 can be related to reversible decomposition of MeNO 3. XPS shows that surface of SrTiO 3 substituted with K (Cs) is much richer in these elements than the surface of impregnated one. Prepared materials lower the temperature of soot ignition from 530 (inert) to 470 °C for SrTiO 3 and to 302–303 °C for Sr 0.8K 0.2TiO 3 and Sr 0.8K 0.2TiO 3, respectively. Substituted materials are more active in soot combustion than impregnated ones. A mechanism explaining effect of alkali metals nitrate addition to SrTiO 3 on its catalytic activity in soot combustion is proposed. 相似文献
19.
It is known that Curie temperature of barium titanate system can be altered by the substitution of dopants into either A- or B-site. Dopants could pinch transition temperature, lower Curie temperature, and raise the rhombohedral–orthorhombic and orthorhombic–tetragonal phase transition close to room temperature. This isovalent substitution could improve the ferroelectric properties of the BaTiO 3-based system. In this study, barium zirconate titanate Ba(Zr xTi 1−x)O 3 (BZT; x = 0, 0.02, 0.05 and 0.08) ceramics were prepared by conventionally mixed-oxide method. The ferroelectric properties of BZT ceramics were investigated. Increasing Zr content in the BaTiO 3-based compositions caused a decrease in Curie temperature ( Tc). At Tc, the highest relative permittivity of BZT with an addition of 0.08 mol% of Zr was 12,780. The BZT specimens with the additions of 0.05 mol% and 0.08 mol% of Zr presented the remanent polarization at 25 μC/cm 2 and 30 μC/cm 2, respectively. 相似文献
20.
K 2NiF 4-type La 0.2Sr 1.8MnO 4 was synthesized by nitrate (ND) and nitrate/acetate (NAD) decomposition methods as well as solid-state reaction. Single-phase oxide was obtained at 550 °C by the ND method just after the decomposition of Sr(NO 3) 2 and at 1000 °C by the NAD method after the decomposition of SrCO 3. The K 2NiF 4-type oxide was hardly formed by the solid-state reaction. In the La–Sr–Mn system, an intermediate compound of SrCO 3, if present or formed during the decomposition process, interfered with the low-temperature formation of the K 2NiF 4-type oxide because of its high decomposition temperature about 1000 °C. The ND method used only metal nitrates and no starting materials with carbon source, so that the low-temperature synthesis of the K 2NiF 4-type oxide was realized without forming obstinate intermediate compound of SrCO 3. The low-temperature synthesis was possible for La xSr 2−xMnO 4 with the substitution of La (0 < x < 0.5) and not for La 0.2A 1.8MnO 4 (A = Ca and Ba). The effect of A-site cations on the K 2NiF 4-phase formation was discussed from the geometric aspect. 相似文献
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