Boreskov Institute of Catalysis of the Siberian Branch of Russian ...

PL-4CATALYTIC CONVERSION OF HYDROCARBON FUELS:FROM MOLECULAR MODELING TO REACTOR OPTIMIZATIONOlaf DeutschmannInstitute for Chemical Technology and Polymer Chemistry, Universität Karlsruhe (TH)Kaiserstraße 12, 76128 Karlsruhe, Germany, e-mail: deutschmann@kit.edu1. IntroductionCatalytic conversion of hydrocarbon fuels is discussed from several view points:experimental studies, development of homogeneous and heterogeneous reactionsmechanisms, CFD simulations, mathematical optimization of operating conditions andcatalyst laodings, experimental model evaluation, and technical applications. Applicationscover synthesis of basic chemicals and hydrogen and high-temperature fuel cells (SOFC).Understanding and optimization of reactors for high-temperature catalysis require theknowledge of the physical and chemical processes on a molecular level. In particular, due toshort contact times and high temperatures, at which reactions occur on the catalyst and in thegas-phase, the interaction of transport and chemistry becomes important. Recently, hightemperaturecatalysis has been extensively discussed, in particular in the light of the synthesisof basic chemicals and hydrogen, and high-temperature fuel cells. Catalytic partial oxidationand autothermal reforming of natural gas, higher alkanes, diesel surrogates, and alcohols overnoble metal catalysts at short contact times offer promising routes for the production ofsynthesis gas [1] , olefins [2] , and hydrogen. High-temperature catalysis is also present in solidoxide fuel cell (SOFC) operated at 800 °C. For any fuel other than hydrogen, catalyticreactions are likely to occur in the anode of a SOFC leading to a complex chemicalcomposition at the anode-electrolyte interface [3] . Today, the challenge in catalysis is not onlythe development of new catalysts to synthesize a desired product, but also the understandingof the interaction of the catalyst with the surrounding reactive flow field. Sometimes, theexploitation of these interactions can lead to the desired product selectivity and yield.2. Reaction mechanisms and coupling to the reactive flow fieldThe development of a reliable surface reaction mechanism is a complex process. Areaction mechanism should include all possible paths for the formation of the chemicalspecies under consideration in order to be «elementary-like» and thus applicable over a widerange of conditions. The mechanism needs to be evaluated by numerous experimentallyderived data, which are compared with theoretical predictions based on the mechanism. Here,the simulations of the laboratory reactors require appropriate models for all significant11