Thin-layer carbon supported Nafion-H catalysts were found to be active and highly selective (S>98%) for the partial oxidation of C1-C3 alkanes, in a three phase catalytic membrane reactor (3PCMR), under mild conditions and in the presence of H2O2. The influences of the catalyst teflon loading and H2O2 concentration on the reaction rate have been evaluated. A reaction pathway, based on the electrophilic hydroxylation of the C-H bond of alkanes with protonated hydrogen peroxide (H3O
2+
), is discussed. 相似文献
Gas-phase selective oxidation of toluene has been carried out on vanadium oxide systems (5–20 wt.% of V2O5, equivalent to 0.4–1.7 theoretical monolayers) supported on TiO2–sepiolite (with titania loading around the theoretical monolayer, 12 wt.%) and on sepiolite. A study has been made on both the influence of vanadia loading and of the support on the catalytic behaviour of the supported vanadium systems. The reducibility by H2 TPR was also studied as well as the acid and basic/redox sites from the results of conversion of the 2-propanol test reaction of the solids. Benzaldehyde, benzoic acid and several coupling products were the main ones detected, attaining over 50% selectivity towards the benzaldehyde and benzoic acid products at a total conversion around 10%. The activity and selectivity to the selective products exhibited by vanadium systems supported on mixed support were superior to those exhibited by the systems supported on sepiolite and increased notably in both series with the increase in vanadium loading. The best catalytic behaviour exhibited by the vanadium systems supported on mixed support, which also exhibited the highest density of sites capable of being reduced (as well as their reducibility) and of those responsible for propanone formation, could be attributed not only to the different balance of the vanadia species existing in the two supports (monomeric + oligomeric/polymeric), but also to such other factors as the nature of the support and, concretely, its chemical composition. 相似文献
A promising catalytic system for the low temperature oxidation of methane to a methanol derivative has been investigated under both batch and semi-continuous operation in two different reactor types. The system comprises of a bimetallic palladium and copper(II) chloride catalyst contained in a trifluoroacetic acid (TFA) and an aqueous phase. Methane, oxygen and a co-reductant carbon monoxide constitute the gas phase. Typical operating conditions were a temperature of 85 °C and a pressure of 83 bar.
The yields of the methyl trifluoroacetate product observed in this present work were less than those obtained in other batch autoclave works, which employed only 4 ml of liquid phase, compared with 50 ml in this study. Furthermore, an encouraging initial product formation rate of ca. 40 mol/m3 h, quickly decreased after the first hour, and came to an apparent end after only 2 h. This observation had not been reported previously.
Work performed in a semi-continuous porous tube reactor (300 ml of re-circulating liquid phase) also showed the same reaction characteristics as in the batch reactor. Thus, the deteriorating product formation rate cannot be attributed to gaseous reactant depletion (batch operation). The results suggest problems associated with catalyst instabilities, e.g. with the previously elucidated Wacker chemistry. 相似文献
Over the last decade, computer supported cooperative work (CSCW) has emerged as an identifiable research area that focuses on the role of the computer in group work. CSCW is a generic term which combines the understanding of the nature of group working with the enabling technologies of computer networking, systems support and applications. The paper examines the classes of system which have emerged to support cooperative working. A framework for characterising and describing CSCW systems is presented and four major classes of cooperative system identified. Each of these classes of cooperative system are examined highlighting their general characteristics and applicability to CSCW. 相似文献
Aqueous solutions of butyric acid were treated by catalytic wet air oxidation using carbon-supported iridium catalysts in a stirred reactor. Under the operating conditions of 6.9 bar of oxygen partial pressure and 200 °C of temperature, conversions up to 52.9% after 2 h were obtained depending on the type of catalyst used. The effects of butyric acid initial concentration, loading of catalyst, oxygen partial pressure and temperature were investigated and the empirical rate law for acid conversion is presented. Oxidation intermediates such as propionic and acetic acid were identified. The heterogeneous catalyzed free-radical oxidation of butyric acid is discussed. 相似文献