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71.
Hydrogen-deuterium exchange in methanol over Al2,O3, platinum black and alumina supported platinum catalysts have been investigated by means of mass spectrometry. The hydrogen-deuterium exchange proceeds faster over Pt/Al2O3 than either platinum black or alumina, and the rate (as well as the rate of dimethyl ether formation) increases with platinum dispersion. From the reactions CH3OH + D2, CD3OH + H2 and CD3OH + D2 the different exchange rates of the CH3 and OH groups (R1, and R2, respectively) were determined. For all catalysts studied the exchange in the OH group was two or three orders of magnitude faster than CH3 group. Exchange in the methyl group needs higher activation energy: R1/R2 ratio increases with temperature. Catalyst pretreatment has an important effect: higher activation temperature results in a higher R1/R2 ratio.
A methematical method is suggested for the evaluation of exchange rates of a molecule with two different types of hydrogen and a model is given for the interpretation of measured data: methanol is activated mainly on Al2,O3, forming surface methoxide groups on the Lewis acidic sites. This methoxide can react with deuterium atoms having been activated over platinum sites. With increasing dispersion the metal-support interface is enhanced which leads to higher rate of exchange. 相似文献
A methematical method is suggested for the evaluation of exchange rates of a molecule with two different types of hydrogen and a model is given for the interpretation of measured data: methanol is activated mainly on Al2,O3, forming surface methoxide groups on the Lewis acidic sites. This methoxide can react with deuterium atoms having been activated over platinum sites. With increasing dispersion the metal-support interface is enhanced which leads to higher rate of exchange. 相似文献
72.
Riccardo Carli Raymond Le Van Mao Claudia L. Blanchi Vittorio Ragaini 《Catalysis Letters》1993,21(3-4):265-274
Gallium species which were incorporated initially in the oxide form, were all in the (+3) oxidation state in the hybrid catalyst and exhibited two types of hydrogen chemisorption sites, shw and shs. The stronger sorption sites shs which predominated at higher gallium dispersion, corresponded probably to the most effective surface configuration for gallium in the aromatization ofn-butane. 相似文献
73.
The concept of non-faradaic electrochemical modification of catalytic activity (NEMCA) has been applied for the in situ control of catalytic activity of a rhodium film deposited on YSZ (yttria stabilized zirconia) solid electrolyte towards reduction of 1000 ppm NO by 1000 ppm C3H6 in presence of excess (5000 ppm) O2 at 300 °C. A temporary heating at this feed composition results in a long-lasting deactivation of the catalyst under open circuit conditions due to partial oxidation of the rhodium surface. Positive current application (5 A) over both the active and the deactivated catalysts gives rise to an enhancement of N2 and CO2 production, the latter exceeding several hundred times the faradaic rate. While active rhodium exhibits a reversible behaviour, electrochemical promotion on the deactivated catalyst is composed of a reversible and an irreversible part. The reversible promotion results from the steady-state accumulation of current-generated active species at the gas exposed catalyst surface whereas the irreversible effect is due to the progressive reduction of the catalyst resulting in an increased recovery rate of lost catalytic activity. The results are encouraging with respect to application of rhodium for the catalytic removal of NO from auto-exhaust gases under lean-burn conditions. 相似文献
74.
Stakheev A. Yu. Gabrielsson P. Gekas I. Teleguina N. S. Bragina G. O. Tolkachev N. N. Baeva G. N. 《Topics in Catalysis》2007,42(1-4):143-147
Pt/Al2O3 and Pt/BaO/Al2O3 catalysts (1 wt% Pt, 10 wt%BaO) were sulfated under conditions simulating a real NSR catalyst operation. Comparative TPR
and XPS studies of sulfur removal from Pt/Al2O3 and Pt/BaO/Al2O3 catalysts indicate that the sulfur removal from Al2O3 surface precedes reductive decomposition of BaSO4 (250–400 °C). Barium sulfate decomposition started with further increase in desulfation temperature at the point of surface
atomic ratio Ba:S = 1 (~450o). Simultaneously, an intensive formation of sulfide species on the catalyst surface was observed. Thermodynamic analysis
of the desulfation process allows us to hypothesize that barium sulfide formation may hinder sulfur removal under reducing
conditions. 相似文献
75.
碳四烷烃催化裂解制低碳烯烃的研究进展 总被引:11,自引:0,他引:11
论述了碳四烷烃催化裂解制低碳烯烃的催化剂体系、影响因素及催化裂解方式。该催化剂体系包括硅铝酸盐及锆硫酸盐,氧化铝与碱金属或碱土金属的混合物,负载型催化剂等3种类型。其中分子筛(晶体硅铝酸盐)及其改性催化剂是研究开发的主要方向。除操作条件外,稀释剂、引发和抑制剂和裂解反应方式对催化裂解反应均有影响。催化裂解反应机理与催化剂的种类和反应条件相关。对于酸性分子筛催化剂有2种比较公认的机理:正碳离子机理,自由基与正碳离子机理两种形式。研究表明碳四烷烃,特别是正丁烷催化裂解制低碳烯烃具有良好的低碳烯烃收率,收率可达50%以上。 相似文献
76.
The adsorption of ethene and propene on titania and titania-supported rhodium has been studied, observing a continuous adsorption even after 24 h. The samples have been reduced at 623 or 773 K, but no difference was observed, whichever the reduction temperature or the presence of rhodium, on the amount of gas adsorbed per unit of surface area of the solid. A study of the polymerization has been done following the equal reactivity hypothesis, and it has been concluded that the role played by the rhodium particles is to facilitate adsorption of the gaseous molecule, that is then transfered to the surface of the support, where it polymerizes. 相似文献
77.
The kinetics of the methanation of carbon dioxide was investigated using an alumina supported Ni-La2O2 catalyst in a differential and integral reactor. In the differential reactor the molar ratio of H2 to CO2 was varied from 0.6 to 30. In the integral reactor the rates were measured with up to 90% conversion. Both reactor tests were carried out at temperatures between 513 and 593 K. The experimental results were described by a Langmuir-Hinshelwood type equation. The kinetics can be explained by assuming equilibrium of dissociative carbon dioxide and hydrogen adsorption, and assuming hydrogenation of surface carbon as the rate determining step. 相似文献
78.
全国48家化肥催化剂制造厂总能力为57Kt/a,产量近30kt/a,设备利用率不到50%。平均万吨氨耗催化剂10.36t,高于国外5.60t水平。现生产31个品种203个型号的催化剂中有103种经部级鉴定,但经常使用的约50种。目前化肥催化剂工业水平与国外相比还存在四方面差距。 相似文献
79.
80.
The effects of oxidation/reduction regeneration treatments, with and without 1,2-dichloropropane present as a chlorinating agent, on the structure of Pt(3%)–Sn(4.5%)/Al2O3 catalysts have been correlated with selectivities for butane/H2 reactions. Particles of Pt0 fin Cl-free catalysts were partly covered by Sn0, but retained exposed ensembles of Pt atoms which were active for isomerisation, hydrogenolysis and dehydrogenation reactions, the latter becoming dominant at high reaction temperatures. Coking reduced Pt ensemble size and, hence, also favoured high selectivities for dehydrogenation as hydrogenolysis and isomerisation sites became poisoned. In contrast, the addition of 1,2-dichloropropane in an oxychlorination step before reduction promoted 1:1 Pt0–Sn0 alloy formation after reduction, the proportion of the total Pt in alloy being enhanced by increasing 1,2-dichloropropane concentration and oxychlorination temperature. The alloy surfaces were inactive for isomerisation and hydrogenolysis reactions, giving dehydrogenation as the sole catalytic reaction. 相似文献