Three-Way Catalysts in a Hybrid Drive System:
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1 Diss. ETH No 105i5 Three-Way Catalysts in a Hybrid Drive System: Experimental Study and Kinetic Modelling A dissertation submitted to the SWISS FEDERAL INSTITUTE OF TECHNOLOGY ZURICH for the degree of Doctor of Technical Sciences presented by Lukas Padeste Dipl. Chem.-Ing. ETH born March 3,1965 citizen of Horgen (ZH) accepted on the recommendation of Prof. Dr. A. Baiker, examiner Prof. Dr. M. K. Eberle, co-examiner 1994
2 Summary The suitability of non-promoted and ceria-promoted Pt-Rh/Al203 catalysts for the exhaust gas control of a hybrid drive system (ETH Hybrid III) has been tested. The heart of this parallel hybrid system is a flywheel providing a short-term energy storage, connected via a continuous variable transmission. This configuration permits charging of the flywheel by the combustion engine which is operated in an intermittent mode. A good efficiency is attained because the operating conditions of the combustion engine can be chosen independently from the speed of the vehicle. In addition an efficient recuperation of the breaking energy is enabled. The intermittent operation mode of the combustion engine leads to a pulsed-flow operation of the catalytic converter. Because air will always enter into the cylinders during shut-down and start-up of the combustion engine, an air plug precedes the exhaust gas pulse. The objective of this study was to gain information about the dynamic behaviour of three-way catalysts under dynamic operation, especially under pulsed-flow operation. Special attention was given to studying the influence of the air plug on the performance of the different catalysts. Dynamic experiments with periodic changes of the feed stoichiometry (^-cycling) and pulsed-flow operation have been performed to simulate the intermittent operation mode of the combustion engine. The tests indicated that ceria-promoted Pt-Rh/Al203 is more suitable under these operating conditions. With the ceria-containing catalyst A,-cycling frequencies up to three times lower could be used without any loss of performance. The benefits of ^.-cycling were higher C3H8 and N0X conversions and lower N2O
3 production at temperatures below 350 C. Exposure of both catalysts to air, as occurs during engine start-up (filling of cylinders with air), resulted in low N0X and C3H8 conversions which were maintained under subsequent stoichiometric operation. Conversions were only improved after exposure of the oxygen loaded catalyst to a fuel-rich exhaust gas. The Pt-Rh/Ce02-Al203 catalyst showed a good performance under pulsed-flow operation when suitable operating conditions were ensured. To allow an efficient control of the A.-value during pulsedflow operation a kinetic model has been developed. The model was used to describe the dynamic behaviour of a honeycomb Pt-Rh/Ce02-Al203 catalyst in an integral reactor during exposure to a simulated exhaust gas. The model was based on Langmuir-Hinshelwood kinetics of the CO oxidation and modified by the introduction of CO and O2 equivalents to mimic an exhaust gas containing CO, H2, 02, NO, C3H6, C3H8, CO2, H20 and N2. A good agreement of experimental with calculated data was obtained for experiments with cycled X.-value and pulsed flow in the temperature range between 200 C and 600 C. The model made it possible to find the optimal operating conditions for eliminating the detrimental effect of the air plug passing through the catalytic converter upon engine start-up.
4 Zusammenfassung Ein unpromotierter und ein mit Ceroxid promotierter Pt-Rh/Al203-Katalysator wurden fiir den Einsatz in der Abgasnachbehandlung eines Fahrzeuges mit Hybridantrieb (ETH Hybrid III) untersucht. Das Herzstiick dieses parallelen Hybridkonzeptes bildet ein Kurzzeitenergiespeicher (Schwungrad), gekoppelt mit einem stufenlosen Getriebe. Diese Anordnung ermbglicht es, das Schwungrad mit dem intermittierend betriebenen Ottomotor (Taktbetrieb) mit optimalem Wirkungsgrad zu laden, da der Betriebspunkt des Motors unabhangig von der Fahrzeuggeschwindigkeit gewahlt werden kann. Ausserdem ist mit dem Schwungrad eine Rekuperation eines grossen Teils der Bremsenergie moglich. Der Taktbetrieb kann sich jedoch nachteilig auf das Verhalten des Katalysators auswirken. Da beim Abstellen und Starten des Verbrennungsmotors Luft in die Zylinder eindringt, geht dem eigentlichen Abgasstrom ein Luftpfropfen voraus. Ziel dieser Arbeit war es, das Verhalten der Dreiwegkatalysatoren im dynamischen Betrieb, speziell im Taktbetrieb, zu untersuchen. Besondere Aufmerksamkeit gait dabei dem Einfluss des Luftpfropfens auf das Umsatzverhalten und die Zusammensetzung der Abgase bei beiden Katalysatoren. Dynamische Experimente mit periodisch wechselnder Abgasstochiometrie (X,-Cycling) und, um den Taktbetrieb des Verbrennungsmotors zu simulieren, mit gepulstem Abgasstrom wurden durchgefuhrt. Die Experimente zeigten, dass der mit Ceroxid promotierte Pt-Rh/Al203-Katalysator besser fiir diese Betriebsbedingungen geeignet ist. Verglichen mit Pt-Rh/Al203, zeigte
5 Pt-Rh/Ce02-Al203 bei bis zu dreimal tieferen A.-Cyclingfrequenzen keine Einbusse im Umsatzverhalten. Durch ^.-Cycling konnten hohere C3H8- and NOx-Umsatze und eine geringere Lachgasbildung bei Temperaturen unter 350 C erreicht werden. Ein Luftpfropfen (Fallen der Zylinder mit Luft) bewirkte tiefere Umsatze von NOx und C3H8, welche bei anschliessendem stochiometrischen Betrieb tief blieben. Folgte dem Luftpfropfen hingegen ein fettes Abgasgemisch, waren die Umsatze hoher. Unter geeigneten Betriebsbedingungen zeigte der Pt-Rh/Ce02-Al203-Katalysator ein gutes Umsatzverhalten im Taktbetrieb. Um wahrend des Taktbetriebes eine gezielte A.-Regelung zu ermoglichen, wurde ein kinetisches Modell formuliert. Das Modell wurde dazu verwendet, um das dynamische Verhalten des Integralreaktors wahrend des Betriebs mit dem Pt-Rh/Ce02-Al203-Katalysator und einem simulierten Abgasgemisch bestehend aus CO, H2, 02, NO, C3H6, C3H8, C02, H20 und N2 zu beschreiben. Das Modell basierte auf Langmuir-Hinshelwood-Kinetik fiir die CO-Oxidation und wurde modifiziert, indem die einzelnen Komponenten des Abgasgemischs durch CO- und 02-Aequivalente ersetzt wurden. Eine gute Uebereinstimmung zwischen experimentellen und berechneten Daten wurde fiir Experimente mit X-Cycling und gepulstem Abgasstrom in einem Temperaturbereich von 200 C bis 600 C erhalten. Mit dem Modell konnten ausserdem die besten Bedingungen gefunden werden, um den schadlichen Einfluss des Luftpfropfens, der beim Start des Verbrennungsmotors durch den Konverter stromt, weitgehend zu ehminieren.
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