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1.
We have investigated the catalytic behavior of Pt encapsulated TiO2 nanotubes for the water gas shift reaction as well as the hydrogenation of CO. Pt–TiO2 nanotube catalysts were prepared by employing fine fiber shaped crystals of [Pt(NH3)4](HCO3)2 complex as a structure determining template material. The turnover frequencies (TOF) of these nanotube catalysts were more than one order of magnitude larger than conventional impregnation Pt/TiO2 catalysts, and the selectivity for methanol in CO–H2 reaction was extraordinary high compared to the impregnation catalysts. The XPS and XRD analyses of the nanotubes revealed characteristic electronic state of reduced TiO2 (Ti3+ in rutile structure) with zerovalent Pt even after the calcination at 773 K. In WGS reaction, electron rich Ti3+ on the nanotube wall may play an important role to activate water molecules for the oxidation of CO. In CO–H2 reaction, similar promotion effect of Ti3+ species may be operating for selective methanol formation by supplying active OH(a). 相似文献
2.
Fengxiang Yin Shengfu Ji Biaohua Chen Liping Zhao Hui Liu Chengyue Li 《Applied catalysis. B, Environmental》2006,66(3-4):265-273
MnOx–CeO2 mixed oxides prepared by sol–gel method, coprecipitation method and modified coprecipitation method were investigated for the complete oxidation of formaldehyde. Structure analysis by H2-TPR and XPS revealed that there were more Mn4+ species and richer lattice oxygen on the surface of the catalyst prepared by the modified coprecipitation method than those of the catalysts prepared by sol–gel and coprecipitation methods, resulting in much higher catalytic activity toward complete oxidation of formaldehyde. The effect of calcination temperature on the structural features and catalytic behavior of the MnOx–CeO2 mixed oxides prepared by the modified coprecipitation was further examined, and the catalyst calcined at 773 K showed 100% formaldehyde conversion at a temperature as low as 373 K. For the samples calcined below 773 K, no any diffraction peak corresponding to manganese oxides could be detected by XRD measurement due to the formation of MnOx–CeO2 solid solution. While the diffraction peaks corresponding to MnO2 phase in the samples calcined above 773 K were clearly observed, indicating the occurrence of phase segregation between MnO2 and CeO2. Accordingly, it was supposed that the strong interaction between MnOx and CeO2, which depends on the preparation route and the calcination temperature, played a crucial role in determining the catalytic activity toward the complete oxidation of formaldehyde. 相似文献
3.
The selective catalytic reduction (SCR) of NO by hydrocarbon is an efficient way to remove NO emission from lean-burn gasoline and diesel exhaust. In this paper, a thermally and hydrothermally stable Al–Ce-pillared clay (Al–Ce-PILC) was synthesized and then modified by SO42−, whose surface area and average pore diameter calcined at 773 K were 161 m2/g and 12.15 nm, respectively. Copper-impregnated Al–Ce-pillared clay catalyst (Cu/SO42−/Al–Ce-PILC) was applied for the SCR of NO by C3H6 in the presence of oxygen. The catalyst 2 wt% Cu/SO42−/Al–Ce-PILC showed good performance over a broad range of temperature, its maximum conversion of NO was 56% at 623 K and remained as high as 22% at 973 K. Furthermore, the presence of 10% water slightly decreased its activity, and this effect was reversible following the removal of water from the feed. Py-IR results showed SO42− modification greatly enhanced the number and strength of Brönsted acidity on the surface of Cu/SO42−/Al–Ce-PILC, which played a vital role in the improvement of NO conversion. TPR and XPS results indicated that both Cu+ and isolated Cu2+ species existed on the optimal catalyst, mainly Cu+, as Cu content increased to 5 wt%, another species CuO aggregates which facilitated the combustion of C3H6 were formed. 相似文献
4.
Co–Nb2O5–SiO2 catalysts were prepared using three different sol–gel procedures: (i) the colloidal sol–gel method using NbCl5 and SiCl4 as precursors; (ii) the polymeric sol–gel method using niobium ethoxide and tetraethyl-orthosilicate (TEOS); (iii) an intermediate procedure between the colloidal and polymeric sol–gel method in which the precursors were those utilized in the CSG but dissolved in a mixture of anhydrous ethanol and CCl4. In all procedures, the elimination of the solvent carried out between 80 and 110°C was followed by a reduction in hydrogen flow (30 ml min−1) at 773 K. Following these procedures, samples containing 10 wt.% Co and 15 wt.% niobium oxide (expressed as Nb2O5) were obtained. The characterization of the catalysts was performed using various techniques: N2 adsorption and desorption curves at 77 K, NH3- and H2-chemisorption, TPO, XPS, XRD, and solid state 1H MAS-NMR. Hydrogenolysis of butane was evaluated. The low reaction rates are assigned to the effect of the metal size, whereas the isobutane selectivity as well as the relatively high stability is due to the acidity of the support. 相似文献
5.
The electrode reactions of the Np3+/Np couple at liquid Cd and Bi electrodes were investigated by cyclic voltammetry at 723, 773 and 823 K in the LiCl–KCl eutectic melt. It was found that the diffusion of Np3+ in the salt phase was the rate-determining step in the cathodic reaction when the concentration of NpCl3 was less than about 1 wt % and the liquid Cd or Bi phase was not saturated with Np. The redox potentials of the Np3+/Np couple at the liquid Cd electrode at 723, 773 and 823 K were observed to be more positive than those at the Mo electrode by 0.158, 0.140 and 0.126 V, respectively. The potential shift results from a lowering of the activity of Np in the Cd phase according to the formation of the NpCd11 alloy at 723 K and NpCd6 at 773 and 823 K. The redox potentials of the Np3+/Np couple at the liquid Bi electrode at 723, 773 and 823 K were more positive than those at the Mo electrode by 0.427, 0.419 and 0.410 V, respectively, which is attributable to a lowering of the activity of Np in the Bi phase due to the formation of NpBi2. 相似文献
6.
Comparative study of Au/ZrO2 catalysts in CO oxidation and 1,3-butadiene hydrogenation 总被引:1,自引:0,他引:1
This work investigates the effects of Au3+/Au0 ratio or distribution of gold oxidation states in Au/ZrO2 catalysts of different gold loadings (0.01–0.76% Au) on CO oxidation and 1,3-butadiene hydrogenation by regulating the temperature of catalyst calcination (393–673 K) and pre-reduction with hydrogen (473–523 K). The catalysts were prepared by deposition–precipitation and were characterized with elemental analysis, nitrogen adsorption/desorption, TEM, XPS and TPR. The catalytic data showed that the exposed metallic Au0 atoms at the surface of Au particles were not the only catalytic sites for the two reactions, isolated Au3+ ions at the surface of ZrO2, such as those in the catalysts containing no more than 0.08% Au were more active by TOF. For 0.76% Au/ZrO2 catalysts having coexisting Au3+ and Au0, the catalytic activity changed differently with varying the Au3+/Au0 ratio in the two reactions. The highest activity for the CO oxidation reaction was observed over the catalyst of Au3+/Au0 = 0.33. However, catalyst with a higher Au3+/Au0 ratio showed always a higher activity for the hydrogenation reaction; co-existance of Au0 with Au3+ ions lowered the catalyst activity. Moreover, the coexisting Au particles changed the product selectivity of 1,3-butadiene hydrogenation to favor the formation of more trans-2-butene and butane. It is thus suggested that for better control of the catalytic performance of Au catalyst the effect of Au3+/Au0 ratio on catalytic reactions should be investigated in combination with the particle size effect of Au. 相似文献
7.
R. Mariscal S. Rojas A. G mez-Cort s G. Dí az R. P rez J. L. G. Fierro 《Catalysis Today》2002,75(1-4):385-391
ZrO2–TiO2 mixed oxides, prepared using the sol–gel method, were used as supports for platinum catalysts. The effects of catalyst pre-reduction and surface acidity on the performance of Pt/ZT catalysts for the reduction of NO with CH4 were studied. The diffuse reflectance infrared Fourier transformed (DRIFT) spectra of CO adsorbed on the Pt/ZT catalysts, and also on the Pt/T and Pt/Z references, pre-reduced at 773 K in hydrogen, revealed that an SMSI state is developed in the Ti-rich oxide-supported platinum catalysts. However, no shift in the binding energy of Pt 4f7/2 level for Pt/T and Pt deposited on Ti-rich support counterparts pre-reduced at 773 K was found by photoelectron spectroscopy. The DRIFT spectra of the catalysts under the NO+O2 co-adsorption revealed the appearance of nitrite/nitrate species on the surface of the Zr-containing catalysts, which displayed acidic properties, but were almost absent in the Pt/T catalyst. The intensity of these bands reached a maximum for the Pt/ZT(1:1) catalyst, which in turn exhibited a larger specific area. In the absence of oxygen in the feed stream, the NO+CH4 reaction showed DRIFT spectra assigned to surface isocyano species. Since the intensity of this band is higher for the Pt/ZT (9:1) catalyst, it seems that such species are developed at the Pt–support interface. 相似文献
8.
L. N. Ikryannikova A. A. Aksenov G. L. Markaryan G. P. Murav eva B. G. Kostyuk A. N. Kharlanov E. V. Lunina 《Applied Catalysis A: General》2001,210(1-2):225-235
The introduction of trivalent cation — Y3+ or La3+ — into the lattice of CeO2–ZrO2 solid solutions allows to stabilise a cubic structure at low ceria content (30 mol%). The reducibility of the samples has been compared in the experiments of temperature-programmed reduction (TPR). The introduction of lanthanum cations decreases the amount of hydrogen consumed during TPR, while the introduction of yttrium ones increases this value. At the same time, the value of temperature of the maximum speed of reduction (Tmax) is independent on the trivalent dopant. The reducibility of these solid solutions did not change during repeated red–ox treatments at temperature below 1220 K. It is connected with the high thermostability of all systems in this temperature interval. TPR up to 1470 K causes a significant shift of Tmax value to higher temperature and a slight decrease of hydrogen consumption in two to three cycles. It is suggested that this alterations are connected with the sharp decrease of the specific surface area of all samples and partially phase decomposition of CeO2–ZrO2 and Y2O3–CeO2–ZrO2 solid solutions. Raman characterisation of the oxygen sublattice of the fresh samples and of the samples after TPR has been carried out. 相似文献
9.
The effect of Te addition over Mo–V–O catalysts supported on alumina is discussed for the ammoxidation of propane to acrylonitrile. Catalyst composition and atmosphere of activation are evaluated. Catalysts are characterized before and after catalytic reaction by XPS, XRD and in situ Raman spectroscopies. The absence of Te in catalysts formulation and the presence of a high amount of vanadium induce the presence of V5+ species and the formation of V2O5 oxide; associated with a decrease in acrylonitrile selectivity. The presence of Mo-based polyacids structures decreases the selectivity to acrylonitrile. V5+ sites are responsible of propane activation and of the subsequent -H abstraction to form the intermediate propylene. Then, a Mo–V rutile-like structure in which vanadium species are reduced as V4+, is responsible for nitrogen insertion and acrylonitrile formation. The formation of such structure is favoured when Te is added to catalysts and is promoted during propane ammoxidation. 相似文献
10.
Te-Yu Wei Shih-Yuan Lu Yu-Cheng Chang 《Journal of the Chinese Institute of Chemical Engineers》2007,38(5-6):477-481
Tin oxide–silica composite aerogels were successfully prepared with a co-fed precursor sol–gel process. The crystallinity of the tin oxide nanoparticles, embedded in the mesoporous SiO2 network, was improved with increasing the post-reaction thermal treatment temperature. The composite aerogels exhibited a rich photoluminescence (PL) emission contributed by both SnO2 and SiO2. The PL peak of 346 nm was from the near band edge emission of the tin oxide nanoparticles, and the ones located at 310 and 476 nm were attributable to the oxygen deficiencies of the silica network. Three more emission peaks, 387, 432, and 522 nm, were observed, with the 387 nm peak contributed by the oxygen vacancies VO++, the 432 nm peak by the Sn interstitials, and the 522 nm peak by the oxygen vacancies VO+, respectively, of the tin oxide nanoparticles. The intensities of these three defect level emissions were found decreased, as compared to that of the near band edge emission, with increasing the post-reaction thermal treatment temperature as the tin oxide crystallinity improved. 相似文献
11.
C. Otero Are n A. L pez Bellan M. Pe arroya Mentruit M. Rodrí guez Delgado G. Turnes Palomino 《Microporous and mesoporous materials》2000,40(1-3):35-42
Mesoporous γ-Ga2O3 was prepared by calcination (at 773 K) of a gallia gel obtained by adding ammonia to an ethanolic solution of gallium nitrate. The corresponding powder X-ray diffraction pattern was found to be similar to that of γ-alumina; all diffraction lines could be indexed by assuming a cubic spinel-type structure having a lattice parameter a0=0.830 nm. Nitrogen adsorption–desorption at 77 K showed the material to have a BET surface area of 120 m2 g−1 and a most frequent pore radius of 2.1 nm. The surface chemistry was studied by FTIR spectroscopy of adsorbed carbon monoxide at liquid nitrogen temperature. Partially hydroxylated γ-Ga2O3 gave main O–H stretching bands at 3692 and 3637 cm−1. These hydroxyl bands were significantly perturbed by adsorbed CO, thus showing a Brønsted acid character. Lewis acidity was monitored by analyzing the C–O stretching mode of carbon monoxide adsorbed on coordinatively unsaturated Ga3+ ions; main IR absorption bands of Ga3+CO adducts were found at 2220 and 2193 cm−1. 相似文献
12.
Mesostructured MnOx–Cs2O–Al2O3 nanocomposites have been synthesized by reverse microemulsion method combined with hydrothermal treatment and then applied to the catalytic combustion of methane. Compared to impregnation-derived conventional MnOx/Cs2O/Com-Al2O3 catalyst, the microemulsion-derived catalyst showed higher activity and stability for methane combustion. The T10% of the fresh and of the 72 h aged MnxO–Cs2O–Al2O3 were 475 and 490 °C, respectively, recommending it as a potential candidate catalyst for application in hybrid gas turbines. The homogeneous composition of the microemulsion-derived nanocomposite catalyst can hinder the loss of Cs+ and accelerate the formation of Cs–β-alumina phase, ensuring thus higher activity and stability for methane combustion. 相似文献
13.
The oxidation of CH4 over Pt–NiO/δ-Al2O3 has been studied in a fluidised bed reactor as part of a major project on an autothermal (combined oxidation–steam reforming) system for CH4 conversion. The kinetic data were collected between 773 and 893 K and 101 kPa total pressure using CH4 and O2 compositions of 10–35% and 8–30%, respectively. Rate–temperature data were also obtained over alumina-supported monometallic catalysts, Pt and NiO. The bimetallic Pt–NiO system has a lower activation energy (80.8 kJ mol−1) than either Pt (86.45 kJ mol−1) and NiO (103.73 kJ mol−1). The superior performance of the bimetallic catalyst was attributed to chemical synergy. The reaction rate over the Pt–NiO catalyst increased monotonically with CH4 partial pressure but was inhibited by O2. At low partial pressures (<30 kPa), H2O has a detrimental effect on CH4 conversion, whilst above 30 kPa, the rate increased dramatically with water content. 相似文献
14.
CH4/CO2 reforming over La2NiO4 and 10%NiO/CeO2–La2O3 catalysts under the condition of supersonic jet expansion was studied via direct monitoring of the reactants and products using the sensitive technique of cavity ring-down spectroscopy. Vibration–rotational absorption lines of CH4, H2O, CO2 and CO molecules were recorded in the near infrared spectral region. Our results indicated that La2NiO4 is superior to 10%NiO/CeO2–La2O3 in performance. In addition, we observed enhanced reverse-water-gas-shift reaction at augmented reaction temperature. The formation of reaction intermediates was also investigated by means of time-of-flight mass spectrometry and there was the detection of CHx+, OH+ and H+ species. 相似文献
15.
A. Barrera J.A. Montoya M. Viniegra J. Navarrete G. Espinosa A. Vargas P. del Angel G. Prez 《Applied Catalysis A: General》2005,290(1-2):97-109
The catalytic performance of mono- and bimetallic Pd (0.6, 1.0 wt.%)–Pt (0.3 wt.%) catalysts supported on ZrO2 (70, 85 wt.%)–Al2O3 (15, 0 wt.%)–WOx (15 wt.%) prepared by sol–gel was studied in the hydroisomerization of n-hexane. The catalysts were characterized by N2 physisorption, XRD, TPR, XPS, Raman, NMR, and FT-IR of adsorbed pyridine. The preparation of ZrW and ZrAlW mixed oxides by sol–gel favored the high dispersion of WOx and the stabilization of zirconia in the tetragonal phase. The Al incorporation avoided the formation of monoclinic-WO3 bulk phase. The catalysts increased their SBET for about 15% promoted by Al2O3 addition. Various oxidation states of WOx species coexist on the surface of the catalysts after calcination. The structure of the highly dispersed surface WOx species is constituted mainly of isolated monotungstate and two-dimensional mono-oxotungstate species in tetrahedral coordination. The activity of Pd/ZrW catalysts in the hydroisomerization of n-hexane is promoted both with the addition of Al to the ZrW mixed oxide and the addition of Pt to Pd/ZrAlW catalysts. The improvement in the activity of Pd/ZrAlW catalysts is ascribed to a moderated acid strength and acidity, which can be correlated to the coexistence of W6+ and reduced-state WOx species (either W4+ or W0). The addition of Pt to the Pd/ZrAlW catalyst does not modify significantly its acidic character. Selectivity results showed that the catalyst produced 2MP, 3MP and the high octane 2,3-dimethylbutane (2,3-DMB) and 2,2-dimethylbutane (2,2-DMB) isomers. 相似文献
16.
Feg-Wen Chang Hsin-Yin Yu L. Selva Roselin Hsien-Chang Yang 《Applied Catalysis A: General》2005,290(1-2):138-147
Selective production of hydrogen by partial oxidation of methanol (CH3OH + (1/2)O2 → 2H2 + CO2) over Au/TiO2 catalysts, prepared by a deposition–precipitation method, was studied. The catalysts were characterized by XRD, TEM, and XPS analyses. TEM observations show that the Au/TiO2 catalysts exhibit hemispherical gold particles, which are strongly attached to the metal oxide support at their flat planes. The size of the gold particles decreases from 3.5 to 1.9 nm during preparation of the catalysts with the rise in pH from 6 to 9 and increases from 2.9 to 4.3 nm with the rise in calcination temperature up to 673 K. XPS analyses demonstrate that in uncalcined catalysts gold existed in three different states: i.e., metallic gold (Au0), non-metallic gold (Auδ+) and Au2O3, and in catalysts calcined at 573 K only in metallic state. The catalytic activity is strongly dependent on the gold particle size. The catalyst precipitated at pH 8 and uncalcined catalysts show the highest activity for hydrogen generation. The partial pressure of oxygen plays an important role in determining the product distribution. There is no carbon monoxide detected when the O2/CH3OH molar ratio in the feed is 0.3. Both hydrogen selectivity and methanol conversion increase with increasing the reaction temperature. The reaction pathway is suggested to consist of consecutive methanol combustion, partial oxidation and steam reforming. 相似文献
17.
G. Munuera A.R. Gonzalez-Elipe J.P. Espinos A. Muoz J.C. Conesa J. Soria J. Sanz 《Catalysis Today》1988,2(5):663-673
Thermal reduction under ultrahigh vacuum or with H2 of RhCl3/TiO2 precursors up to 773K has been studied either directly or after precalcination with O2 at 773K. The evolution of rhodium and chlorine has been followed with the aid of XPS, EPR, IR 1H-NMR and TPR/DTG for the different treatments. Ar+ sputtering has been used in combination with XPS to examine in detail the incorporation of chlorine to the TiO2 support. A model is proposed which assumes the formation during the reduction process of oxygen vacancies (Vo) associated to Ti3+ species (i.e. (TiVo)n3n+). These centers act promoting the reduction of Rh3+ to Rho and upon extensive reduction at 773K in H2, as anchoring sites of Rho through interaction with exposed Ti3+ ions. Oxygen vacancies sites are also able to incorporate chlorine and hydrogen to form in the later case hydride, (Ti-H)3+, species that we have previously found to have a role in the SMSI state. 相似文献
18.
The local structure and the photoactivity of B2O3–SiO2/TiO2 ternary mixed oxides (SiO2 content was fixed as 30 at.% with respect to TiO2) was investigated by using XRD, FT-IR, BET, UV-vis spectra, and electron paramagnetic resonance (EPR) measurement. In FT-IR analysis, boron was incorporated into the framework of titania matrix with replacing Ti---O---Si with Si---O---B or Ti---O---B bonds. Also, paramagnetic species such as O− and Ti3+ defects were formed by the boron incorporation. In SiO2/TiO2 mixed oxides, a blue shift in the light absorption band was observed due to the quantization of band structure. All B2O3–SiO2/TiO2 samples had pure anatase phase and no rutile phase was formed even though the calcination temperature was over 900 °C. Incorporating boron oxides of more than 10% enlarges the grain size of anatase phase and causes a red shift of the light absorption spectrum. The surface area was monotonically decreased with increasing the content of boron content. As a result, the photoactivity of B2O3–SiO2/TiO2 ternary mixed oxides was greatly influenced by the content of boron oxide. The highest photoactivity (g moles/min l) was obtained when the boron content was 5% and seven times higher than that of silica/titania binary mixed oxide. In addition, the specific photoactivity (g moles/m2 l) was maximum still at 5%. It was concluded that the large reduction of surface area, the change of band structure, and more formation of bulk Ti3+ sites are responsible for the deterioration in the photoactivity of B2O3–SiO2/TiO2 ternary mixed oxides when the content of boron is over 10%, although their crystallinity was enhanced by increasing the calcination temperature with keeping anatase phase. 相似文献
19.
Mohammed A. Amin Sayed S. Abd El Rehim S.O. Moussa Abdallah S. Ellithy 《Electrochimica acta》2008,53(18):5644-5652
The influence of various concentrations of NaClO4, as a pitting corrosion agent, on the corrosion behaviour of pure Al, and two Al–Cu alloys, namely (Al + 2.5 wt% Cu) and (Al + 7 wt% Cu) alloys in 1.0 M Na2SO4 solution was investigated by potentiodynamic polarization and potentiostatic techniques at 25 °C. Measurements were conducted under the influence of various experimental conditions, complemented by ex situ energy dispersive X-ray (EDX) and scanning electron microscopy (SEM) examinations of the electrode surface. In free perchlorate sulphate solutions, for the three Al samples, the anodic polarization exhibits an active/passive transition. The active dissolution region involves an anodic peak (peak A) which is assigned to the formation of Al2O3 passive film on the electrode surface. The passive region extends up to 1500 mV with almost constant current density (jpass) without exhibiting a critical breakdown potential or showing any evidence of pitting attack. For the three Al samples, addition of ClO4− ions to the sulphate solution stimulates their active anodic dissolution and tends to induce pitting corrosion within the oxide passive region. Pitting corrosion was confirmed by SEM examination of the electrode surface. The pitting potential decreases with increasing ClO4− ion concentration indicating a decrease in pitting corrosion resistance. The susceptibility of the three Al samples towards pitting corrosion decreases in the order: Al > (Al + 2.5 wt% Cu) alloy > (Al + 7 wt% Cu) alloy. Potentiostatic measurements showed that the rate of pitting initiation increases with increasing ClO4− ion concentration and applied step anodic potential, while it decreases with increasing %Cu in the Al samples. The inhibitive effect of SO42− ions was also discussed. 相似文献
20.
Xiankuan Zhang Arden B. Walters M. Albert Vannice 《Applied catalysis. B, Environmental》1996,7(3-4):321-336
Both NO decomposition and NO reduction by CH4 over 4%Sr/La2O3 in the absence and presence of O2 were examined between 773 and 973 K, and N2O decomposition was also studied. The presence of CH4 greatly increased the conversion of NO to N2 and this activity was further enhanced by co-fed O2. For example, at 773 K and 15 Torr NO the specific activities of NO decomposition, reduction by CH4 in the absence of O2, and reduction with 1% O2 in the feed were 8.3·10−4, 4.6·10−3, and 1.3·10−2 μmol N2/s m2, respectively. This oxygen-enhanced activity for NO reduction is attributed to the formation of methyl (and/or methylene) species on the oxide surface. NO decomposition on this catalyst occurred with an activation energy of 28 kcal/mol and the reaction order at 923 K with respect to NO was 1.1. The rate of N2 formation by decomposition was inhibited by O2 in the feed even though the reaction order in NO remained the same. The rate of NO reduction by CH4 continuously increased with temperature to 973 K with no bend-over in either the absence or the presence of O2 with equal activation energies of 26 kcal/mol. The addition of O2 increased the reaction order in CH4 at 923 K from 0.19 to 0.87, while it decreased the reaction order in NO from 0.73 to 0.55. The reaction order in O2 was 0.26 up to 0.5% O2 during which time the CH4 concentration was not decreased significantly. N2O decomposition occurs rapidly on this catalyst with a specific activity of 1.6·10−4 μmol N2/s m2 at 623 K and 1220 ppm N2O and an activation energy of 24 kcal/mol. The addition of CH4 inhibits this decomposition reaction. Finally, the use of either CO or H2 as the reductant (no O2) produced specific activities at 773 K that were almost 5 times greater than that with CH4 and gave activation energies of 21–26 kcal/mol, thus demonstrating the potential of using CO/H2 to reduce NO to N2 over these REO catalysts. 相似文献