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Selective hydrogenation of citral with transition metal complexes in supercritical carbon dioxide

Paper ID Volume ID Publish Year Pages File Format Full-Text
43818 45990 2007 7 PDF Available
Title
Selective hydrogenation of citral with transition metal complexes in supercritical carbon dioxide
Abstract

The activity and selectivity of the transition metal complexes formed from Ru, Rh, Pd and Ni with triphenylphosphine (TPP) have been investigated for hydrogenation of citral in supercritical carbon dioxide (scCO2). High activities are obtained with Ru/TPP and Pd/TPP catalysts, and the overall activity is in the order of Pd≈Ru > Rh > Ni. The Ru/TPP complex is highly selective to the formation of unsaturated alcohols of geraniol and nerol. In contrast, the Pd/TPP catalyst is more selective to partially saturated aldehydes of citronellal. Furthermore, the influence of several parameters such as CO2 and H2 pressures, N2 pressure and reaction time has been discussed. CO2 pressure has a significant impact on the product distribution, and the selectivity for geraniol and nerol can be enhanced from 27% to 75% with increasing CO2 pressure from 6 to 16 MPa, while the selectivity for citronellol decreases from 70% to 20%. Striking changes in the conversion and product distribution in scCO2 could be interpreted with variations in the phase behavior and the molecular interaction between CO2 and the substrate in the gas phase and in the liquid phase.

Graphical abstractHigh activities are obtained with Ru/TPP complexes for hydrogenation of citral in supercritical carbon dioxide (scCO2). CO2 pressure has a significant impact on the product selectivity. Striking changes in the conversion and selectivity in scCO2 could be interpreted with the variations in the phase behavior and the molecular interaction between CO2 and the substrate. Figure optionsDownload full-size imageDownload as PowerPoint slide

Keywords
Selective hydrogenation; Citral; Transition metal complexes; Supercritical carbon dioxide; Phase behavior
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volume 316, Issue 2, 10 January 2007, Pages 127–133
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
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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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