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- W2023170629 abstract "Laser Initiated Homogeneous Catalysis: Kinetics of Elementary ReactionsMichael E. Miller and Edward R. GrantDepartment of Chemistry, Cornell UniversityIthaca, New York 14853AbstractThe gas phase hydrogenation of ethylene is homogeneously photocatalyzed by pulsed ex-cimer laser irradiation of iron pentacarbonyl in situ. The experiments, performed undermild conditions of temperature (10 -70 °C) and total pressure (1 -2.4 atm), result in quantumyields (defined as the number of product molecules formed per single photon absorbed) ashigh as 170. This efficiency per photon is much greater than unity in every measurement.The laser initiates catalytic activity with temporally distinct bursts of light, whichallows most of the catalyst to revert to an inactive species before the next pulse entersthe system. The catalyst generated by the laser light is thermally active, so that ourmethod separates the photochemical initiation from the actual thermal catalysis, providingan opportunity for a detailed study of the elementary reactions involved in the catalyticsystem itself. Varying the pressures of Fe(CO)5, ethylene, and hydrogen gives relativerates of steps within the cycle, while changing the time between successive laser pulsesyields the average lifetime of the catalyst. Controlled temperature experiments revealactivation energies for more than one step in the catalyzed hydrogenation system.IntroductionHomogeneous photocatalysis by transition metal organometallics efficiently promotes awide variety of liquid phase organic reactions.1 Studies on such reactions have offerednew routes to important chemical intermediates and final products and provided clues aboutthe basic mechanisms of catalytic activity.2 We have recently demonstrated that entirelyanalogous photocatalytic behavior can be initiated by pulsed UV laser radiation in homo-geneous gas phase systems.3 This development has important kinetic and dynamical implica-" @default.
- W2023170629 created "2016-06-24" @default.
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- W2023170629 date "1984-05-31" @default.
- W2023170629 modified "2023-09-23" @default.
- W2023170629 title "Laser Initiated Homogeneous Catalysis: Kinetics Of Elementary Reactions" @default.
- W2023170629 doi "https://doi.org/10.1117/12.939426" @default.
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