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Proceedings Paper

Laser Initiated Homogeneous Catalysis: Kinetics Of Elementary Reactions
Author(s): Michael E. Miller; Edward R Grant
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Paper Abstract

The gas phase hydrogenation of ethylene is homogeneously photocatalyzed by pulsed excimer laser irradiation of iron pentacarbonyl in situ. The experiments, performed under mild conditions of temperature (10-70°C) and total pressure (1-2.4 atm), result in quantum yields (defined as the number of product molecules formed per single photon absorbed) as high 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, which allows most of the catalyst to revert to an inactive species before the next pulse enters the system. The catalyst generated by the laser light is thermally active, so that our method separates the photochemical initiation from the actual thermal catalysis, providing an opportunity for a detailed study of the elementary reactions involved in the catalytic system itself. Varying the pressures of Fe(C0)5, ethylene, and hydrogen gives relative rates of steps within the cycle, while changing the time between successive laser pulses yields the average lifetime of the catalyst. Controlled temperature experiments reveal activation energies for more than one step in the catalyzed hydrogenation system.

Paper Details

Date Published: 31 May 1984
PDF: 5 pages
Proc. SPIE 0458, Applications of Lasers to Industrial Chemistry, (31 May 1984); doi: 10.1117/12.939426
Show Author Affiliations
Michael E. Miller, Cornell University (United States)
Edward R Grant, Cornell University (United States)

Published in SPIE Proceedings Vol. 0458:
Applications of Lasers to Industrial Chemistry
Richard L. Woodin; Andrew Kaldor, Editor(s)

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