Objective
THE AIM OF THIS PROJECT IS TO DEVELOP A NEW ACTIVE AND SELECTIVE CATALYST, BASED MAINLY ON ZEOLITE MOLECULAR SIEVES, FOR THE OXIDATIVE COUPLING OF METHANE TO PRODUCE HIGHER HYDROCARBONS.
Microporous crystalline oxides were evaluated as potential catalyst for the oxidative coupling of methane into higher hydrocarbons (hydrocarbons with chains greater or equal to 2 carbons long, C2+). Without modification, the zeolites and molecular sieves generally exhibited a low C2+ selectivity. The C2+ selectivity can be enhanced considerably by supporting alkaline earth and lanthanide element oxides on zeolite supports. The use of shape selective zeolite catalysts for the conversion of the primary products from oxidative coupling reactions in the gas phase into high yields of aromatics, was demonstrated.
Dense complex crystalline oxides were prepared by the citrate and oxalate methods. Solid solutions of alkaline earth metals and lanthanide element oxides and substituted perovskites prepared by the citrate method showed a superior C2+ selectivity compared to catalysts prepared by conventional methods. The performances of perovskites substituted with alkaline earth metals were comparable to those of alkali metal containing catalysts, but had the advantage that they do not deactivate.
A reaction mechanism for the oxidative coupling of methane on oxide catalysts was deried from oxygen-18 isotope labelling and magic angle spinning nuclear magnetic resonance (MAS NMR) experiments and the reaction kinetics.
Noncatalytic mechanism for the oxidative coupling of methane was performed in an empty reactor tube. The C2+ yields that were obtained in the homogeneous gas phase reactions were only slightly inferior to the yields obtained on the best actually available catalysts. The combination of noncatalytic oxidative coupling with oligomerisation and aromatization over acidic zeolites resulted in the production of liquid C3+ hydrocarbons and aromatics.
THERE ARE INDICATIONS THAT ZEOLITES CAN CATALYZE THE OXIDATIVE COUPLING OF METHANE TO HIGHER HYDROCARBONS TWO CLOSELY COOPERATING CONTRACTORS - THE UNIVERSITIES OF LEUVEN (L GROUP) AND OLDENBURG (O GROUP) - ARE INVOLVED IN THE PROJECT AIMED AT DEVELOPING A ZEOLITE-BASED NEW CATALYST. THE PREPARATION OF A NUMBER OF CATALYST TO UNDERGO SUBSEQUENT SCREENING WILL BE SHARED BETWEEN THE TWO GROUPS ACCORDING TO THEIR SPECIFIC EXPERIENCE. THE FOLLOWING MATERIALS WILL BE SYNTHESIZED:- ZEOLITES OF DIFFERENT CHEMICAL COMPOSITION (SIO2, AL2O3; AL2O3, P2O5; SIO2, AL2O3, P2O5; TIO2, AL2O3, P2O5), I.E. OF DIFFERENT ACID-BASE PROPERTIES, AND OF DIFFERENT PORE SIZE, SHAPE AND DISTRIBUTION.
SUBSEQUENT MODIFICATIONS OF THESE ZEOLITES BY TECHNIQUES SUCH AS ION EXCHANGE, DEALUMINIZATION, IMPREGNATION OR A COMBINATION THEREOF LEADING TO THE INTRODUCTION OF MO, BI, SB, PB IONS WILL BE CARRIED OUT BY O GROUP. AMORPHOUS POLYOXIDES VIA PRECIPITATION, CO-PRECIPITATION, ETC. MIXED AMORPHOUS POLYOXIDES AND ZEOLITES, NEAT OR MODIFIED AS INDICATED. SCREENING OF THE ABOVE MENTIONED CATALYSTS WILL THEN BE CARRIED OUT AT ATMOSPHERIC PRESSURE (L GROUP) IN A PURPOSE-BUILT, CONTINUOUS-FLOW, FULLY AUTOMATED APPARATUS CONNECTED ON-LINE TO A GAS CHROMATOGRAPH AND PROCESS COMPUTER. METHANE IN EXCESS OF THE OXYGEN AND TEMPERATURES IN THE RAGE 650 TO 850 CELSIUS DEGREES WILL BE USED. ON SELECTED CATALYSTS, HIGH PRESSURE TESTS (UP TO 10 MPA) WILL BE PERFORMED (O GROUP) IN AN ANALOGOUS SYSTEM. THE BEST-PERFORMING CATALYSTS WILL UNDERGO OPTIMIZATION WITH RESPECT BOTH TO THEIR COMPOSITION AND TO REACTION CONDITIONS. A THOROUGH STUDY, WITH LABELLED REACTANTS, WILL FINALLY BE PERFORMED BY L GROUP ON A SELECTIVE CATALYST TO ELUCIDATE THE REACTION MECHANISM. AN EXTENSIVE KINETIC STUDY ON A SELECTED CATALYST WILL BE PERFORMED BY O GROUP IN THE HIGH-PRESSURE REACTOR WITH A VIEW TO MAKING A SELECTION FROM AMONG SEVERAL MATHEMATICAL MODELS. A RELIABLE MODEL TO SERVE AS A BASIS FOR THE PROCESS DESIGN WILL THEN BE MADE AVAILABLE.
Fields of science (EuroSciVoc)
CORDIS classifies projects with EuroSciVoc, a multilingual taxonomy of fields of science, through a semi-automatic process based on NLP techniques. See: The European Science Vocabulary.
CORDIS classifies projects with EuroSciVoc, a multilingual taxonomy of fields of science, through a semi-automatic process based on NLP techniques. See: The European Science Vocabulary.
- natural sciences chemical sciences inorganic chemistry inorganic compounds
- natural sciences chemical sciences inorganic chemistry alkaline earth metals
- natural sciences chemical sciences organic chemistry hydrocarbons
- natural sciences chemical sciences catalysis
- natural sciences chemical sciences organic chemistry aliphatic compounds
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Coordinator
3000 LOUVAIN / LEUVEN
Belgium
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