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排序方式: 共有251条查询结果,搜索用时 15 毫秒
1.
应用静态吸附、动态吸附、程序升温脱附和程序升温还原等实验方法,考察了噻吩在Ni基非晶态合金上的吸附和脱附行为。常温下,噻吩分子首先吸附在清洁的Ni表面,并立刻被活化,发生氢解反应,C-S键断裂,释放出烃类部分,S留在Ni原子上。噻吩可以在Ni基非晶态合金表面发生强度不同的化学吸附。弱化学吸附的噻吩可以脱附;强化学吸附的噻吩不会脱附,而在高温下发生氢解反应。 相似文献
2.
The role of Ag in simultaneously catalyzing NO reduction and C3H6 oxidation was shown to be strongly dependent on the redox properties of its local environment. Under an atmosphere of 1,000 ppm
NO, 3,000 ppm C3H6, and 1% O2 and a GHSV of 30,000 h−1, a perovskite La0.88Ag0.12FeO3 prepared by reactive grinding is active giving a complete NO conversion and 92% C3H6 conversion at 500 °C. These values are much higher than the NO conversion of 55% and C3H6 conversion of 45% obtained over a 3 wt.% Ag/Al2O3 catalyst under the same conditions. Under an excess of oxygen (10% O2) a good SCR performance with a plateau of N2 yield above 97% over a wide temperature window of 350–500 °C along with C3H6 conversion of 90% at 500 °C was observed over Ag/Al2O3, while minor N2 yields (∼10% at 250–350 °C) and high C3H6 conversions (reaching ∼100% at 450 °C) were obtained over La0.88Ag0.12FeO3. Abundant molecular oxygen is desorbed from Ag substituted perovskite after 10% O2 adsorption as verified by O2- temperature programmed desorption (TPD). This reflects the strongly oxidative properties of La0.88Ag0.12FeO3, which lead to a satisfactory NO reduction at 1% O2 due to the ease of nitrate formation but to a significant C3H6 combustion above that value. The formation of nitrate species over the less oxidizing Ag/Al2O3 was accelerated under an excess of oxygen resulting in an excellent lean NO reduction behavior. The redox properties of silver
catalysts could be adjusted via mixing perovskite with alumina for an optimal elimination of both NO and C3H6 over the whole range of oxygen concentration between 0 to 10%. 相似文献
3.
The adsorption properties of oxygen and methane on Ga-ZSM-5 and Cu-ZSM-5 catalysts were examined by a TPD method to clarify the extraordinary selectivity of HC-SCR using methane on Ga-ZSM-5. It was observed that Ga-ZSM-5 did not adsorb oxygen but adsorbed methane dissociatively, while on Cu-ZSM-5 oxygen was dissociatively adsorbed and reacted with adsorbed ethylene. 相似文献
4.
Isothermal storage of NO2 and subsequent reduction with different reducing agents (H2, CO or H2 + CO) in a lean NO
x
trap catalyst was tested by Temperature Programmed Desorption (TPD) and Temperature Programmed Reduction (TPR) experiments
at temperatures representative of automotive “cold-start” conditions (<200 °C) using a commercial NO
x
trap catalyst.
Results from the TPR experiments revealed that no reduction of stored NO2 to N2 was observed at 100–180 °C, and at 200 °C 10% reduction only of NO2 to N2 was measured.
A special affinity of H2 to form NH3 was observed during the reduction of stored NO2. The formation of NH3 increases with increasing amount of stored NO2 and decreases with increasing storage temperature. Direct relation exists between the amount of adsorbed and/or stored NO2 and the formation of H2O and NH3. 相似文献
5.
Abdullahi Nuhu Jorge Soares Monica Gonzalez-Herrera Andrew Watts Ghulam Hussein Michael Bowker 《Topics in Catalysis》2007,44(1-2):293-297
We have investigated the adsorption and reaction of methanol with Au/TiO2 catalysts using a pulsed flow reactor, DRIFTS and TPD. The TiO2 (P25) surface adsorbed a full monolayer of methanol, much of it in a dissociative manner, forming methoxy groups associated
with the cationic sites, and hydroxyl groups at the anions. The methoxy is relatively stable until 250 °C, at which point
decomposition occurs, producing mainly dimethyl ether by a bimolecular surface reaction. As the concentration of methoxy on
the surface diminishes, so the mechanism reverts to a de-oxygenation pathway, producing mainly methane and water (at ~330 °C
in TPD), but also with some coincident CO and hydrogen. Au catalysts were prepared by the deposition-precipitation method
to give Au loadings between 0.5–3 wt %. The effect of low levels of Au on the reactivity is marked. The pathway which gives
methane, which is characteristic of titania, remains, but a new feature of the reaction is the evolution of CO2 and H2 at lower temperature (a peak is seen in TPD at 220 °C), and the elimination of the DME-producing state. Clearly this is associated
with the presence of Au and appears to be due to the production of a formate species on the surface of the Au component. This
formate species is mainly involved in the reaction of methanol with the Au/TiO2 catalysts which results in a combustion pathway being followed, with complete conversion occurring by ~130 °C. 相似文献
6.
Ni–W catalysts were prepared by impregnation of commercial -alumina and silica supports. The sulfidation, performed directly after drying at 100°C, yielded fully sulfided Ni–W species on both supports (SEM-EDAX, XPS, XRD). At optimal metals loading (50 wt% NiO + WO3, Ni/W = 2), the sulfided catalysts had similar texture (N2 adsorption) and displayed similar activity in dibenzothiophene hydrodesulfurization (DBT HDS), while the activity of the Ni–W/SiO2 catalyst in toluene hydrogenation (HYD) was six times higher than that of Ni–W/Al2O3. This is due to the more than two times higher WS2 slabs stacking number in Ni–W/SiO2 compared with Ni–W/Al2O3 (XRD, HR-TEM), yielding stronger adsorption of toluene (TPD). 相似文献
7.
The causes of the deactivation of catalysts for fuel combustion MeCr2O4/ -Al2O3 (Me = Cu or Mg) have been investigated using a variety of complex physical-chemical methods: IRS, ESDR, XPS, TPD and a pulse microcatalytic method. It has been concluded that the observed deactivation of catalysts during fuel combustion is due to the combined effect of high temperatures and reduction media. 相似文献
8.
George G. Olympiou Christos M. Kalamaras Constantinos D. Zeinalipour-Yazdi Angelos M. Efstathiou 《Catalysis Today》2007,127(1-4):304-318
Steady-state isotopic transient kinetic analysis (SSITKA) experiments coupled with mass spectrometry were performed for the first time to study essential mechanistic aspects of the water–gas shift (WGS) reaction over alumina-supported Pt, Pd, and Rh catalysts. In particular, the concentrations (μmol g−1) of active intermediate species found in the carbon-path from CO to the CO2 product gas (use of 13CO), and in the hydrogen-path from H2O to the H2 product gas (use of D2O) of the reaction mechanism were determined. It was found that by increasing the reaction temperature from 350 to 500 °C the concentration of active species in both the carbon-path and hydrogen-path increased significantly. Based on the large concentration of active species present in the hydrogen-path (OH/H located on the alumina support), the latter being larger than six equivalent monolayers based on the exposed noble metal surface area (θ > 6.0), the small concentration of OH groups along the periphery of metal-support interface, and the significantly smaller concentration (μmol g−1) of active species present in the carbon-path (adsorbed CO on the noble metal and COOH species on the alumina support and/or the metal-support interface), it might be suggested that diffusion of OH/H species on the alumina support towards catalytic sites present in the hydrogen-path of reaction mechanism might be considered as a slow reaction step. The formation of labile OH/H species is the result of dissociative chemisorption of water on the alumina support, where the role of noble metal is to activate the CO chemisorption and likely to promote formate decomposition into CO2 and H2 products. It was found that there is a good correlation between the surface concentration and binding energy of CO on the noble metal (Pt, Pd or Rh) with the activity of alumina-supported noble metal towards the WGS reaction. 相似文献
9.
Yuko Habuta Naoaki Narishige Kazu Okumura Naonobu Katada Miki Niwa 《Catalysis Today》2003,78(1-4):131-138
Vanadium oxide spread highly on TiO2 (anatase, A) and SnO2, and rather densely on TiO2 (rutile, R) and ZrO2 to make the monolayer in less than 4–5 V nm−2. Profile of acid site of the monolayer was measured by temperature programmed desorption of ammonia, and its relation with the surface oxidation state was studied. The acid site density was high on the V2O5/TiO2 (A) independent of the degree of oxidation. On the other hand, that of V2O5/TiO2 (R) and V2O5/ZrO2 depended on the oxidation state, and the high value of the concentration was observed on the oxidized one. The strength of acid site generated on the V2O5 monolayer on TiO2 was as high as on the HZSM-5 zeolite. Turnover frequency (TOF) of propane conversion, and product selectivity were measured in propane oxidation. Among tested oxides, the V2O5/TiO2 (A) showed the high TOF and selectivity to form propylene, while those loaded on TiO2 (R) and ZrO2 the small TOF and poor selectivity. Therefore, the reaction profile of activity and selectivity could be related with the extent of spreading and solid acidity. An idea of limit of the acid site density ca. 1.5 nm−2 on the monolayer was elucidated. 相似文献
10.
Meso-porous Al2O3-supported Ni catalysts exhibited the highest activity, stability and excellent coke-resistance ability for CH4 reforming with CO2 among several oxide-supported Ni catalysts (meso-porous Al2O3 (Yas1-2, Yas3-8), -Al2O3, -Al2O3, SiO2, MgO, La2O3, CeO2 and ZrO2). The properties of deposited carbons depended on the properties of the supports, and on the meso-porous Al2O3-supported Ni catalyst, only the intermediate carbon of the reforming reaction formed. XRD and H2-TPR analysis found that mainly spinel NiAl2O4 formed in meso-porous Al2O3 and -Al2O3-supported catalysts, while only NiO was detected in -Al2O3, SiO2, CeO2, La2O3 and ZrO2 supports. The strong interaction between Ni and meso-porous Al2O3 improved the dispersion of Ni, retarded its sintering and improved the activated adsorption of CO2. The coking reaction via CH4 temperature-programed decomposition indicated that meso-porous Al2O3-supported Ni catalysts were less active for carbon formation by CH4 decomposition than Ni/-Al2O3 and Ni/-Al2O3. 相似文献