Collaborative Research Centre 546

"Structure, Dynamics and Reactivity of Aggregates of Transition Metal Oxides"


Project B3


General information
 
Title:  Dehydrogenation and partial oxidation of short alkanes

Research areas: Heterogeneous catalysis

Leader:
 
 
 
 
 

 

Dr. Uwe Dingerdissen

Institut für Angewandte Chemie Adlershof e.V.
Richard-Willstätter-Str.12
12489 Berlin
Telefon: 030 6392 4444
Telefax: 030 8413 4454
E-Mail-Adresse: dingerdissen@aca-berlin.de

Dr. Evgenii Kondratenko

Institut für Angewandte Chemie Adlershof e.V.
Richard-Willstätter-Str.12
12489 Berlin
Telefon: 030 6392 4448
Telefax: 030 8413 4454
E-Mail-Adresse: evgenii@aca-berlin.de

Abstract:

During the previous period, it was shown that higher propene selectivity in the oxidative dehydrogenation of propane (ODP) over differently structured VOx species is achieved with N2O as compared to O2 at similar degrees of C3H8 conversion. The positive effect of N2O is related to the inhibition of direct C3H8 oxidation and also the consecutive oxidation of C3H6 to COx. The catalytic activity is, however, lower in the presence of N2O as compared to O2. This is due to the weaker oxidizing potential of N2O relative to O2 for the re-oxidation of the reduced surface VOx sites during the ODP reaction.
In order to further elaborate on the influence of oxidizing agent on certain reaction pathways, the developed methodology should be applied for other catalytic transformations (dehydrogenation, O-insertion and C-C-splitting) of C2-C4 hydrocarbons over more complex catalytic V-Me-Ox (Me=, Te, Mo, Nb) systems. The main aim of the project is to couple mechanistic knowledge of vanadium-catalyzed reactions and structural catalyst characteristics with macroscopic observations in chemical reactor. This knowledge is of highly importance for catalyst or process design.
In order to achieve the above aim, the following strategy will be applied: i) monitoring of catalyst preparation, ii) characterization of catalytic materials under working conditions in particular combining several in-situ techniques to extend the information potential; iii) elucidation of mechanistic and kinetic aspects of heterogeneous reaction steps via steady-state and transient (temporal analysis of products reactor and steady-state isotopic transient kinetic analysis) analysis. A particular attention will be paid to understanding the effect of support on structure, distribution, reactivity and selectivity of VOx species in the oxidative dehydrogenation of propane. The structural information will be obtained in close cooperation with projects B1 and B2. Performance of real catalysts in the ODP reaction will be compared with those obtained for thick vanadia films (project C1) and for well-defined model VOx species over various supports (project B1). In order to derive a comprehensive picture of the catalyst, catalyst preparation will be monitored using in-situ UV/Vis analysis both of solutions of single components and calcination procedure.

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