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Non-equilibrium effects in the hydrogenation-mediated isomerization mechanism of olefins during cavitating ultrasound processing

Paper ID Volume ID Publish Year Pages File Format Full-Text
52996 46895 2006 3 PDF Available
Title
Non-equilibrium effects in the hydrogenation-mediated isomerization mechanism of olefins during cavitating ultrasound processing
Abstract

The process whereby cis-olefins isomerize to their trans form is generally understood as occurring through C–H activation of surface bound alkyl radical species. Here we present aqueous phase deuteration results of cis-2-buten-1-ol on Raney Nickel. In the context of the accepted olefin isomerization mechanism, our results illustrate that transition-state theory can accurately model the competition between C–H and C–D activation for olefin exchange (isomerization) for the case of conventional catalytic processing. This is the case also for a catalytic process that includes cavitating ultrasound, although the model then requires a much higher vibrational temperature (at least ∼800 K) in order to simulate the selectivity of the deuterium exchange process. Thus, cavitating ultrasound likely incorporates a high level of molecular vibrational excitation, suggesting that the vibrational temperature is not in equilibrium with the thermal (e.g., translational) temperature as the chemistry proceeds along a traditional reaction path.

Keywords
Olefin exchange; Hydrogenation; Deuteration; Vibrational temperature; Transition-state theory
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Non-equilibrium effects in the hydrogenation-mediated isomerization mechanism of olefins during cavitating ultrasound processing
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Publisher
Database: Elsevier - ScienceDirect
Journal: Catalysis Communications - Volume 7, Issue 6, June 2006, Pages 348–350
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
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Full-text PDF Download
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