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"Mechanistic Aspects of Dihydrogen Activation and
Transfer During Asymmetric Hydrogenation in Supercritical Carbon Dioxide"
S. Lange, A. Brinkmann, P. Trautner, K.
Woelk, J. Bargon, and W.
Leitner,
Chirality 12, 450-457 (2000).
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A new "CO2-philic" chiral rhodium diphosphinite complex (A)
was synthesized and applied as catalyst precursor in the asymmetric hydrogenation
of dimethyl itaconate in scCO2, scC2H6,
and various liquid organic solvents.
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Deuterium labeling studies and parahydrogen-induced polarization (PHIP)
NMR experiments were used to provide the first detailed mechanistic insight
into the activation and transfer of the diydrogen molecule during hydrogenations
in scCO2.
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Chemical interactions between CO2 and reactive intermediates
were excluded as explanations for the experimentally obtained difference
in the catalytic behavior of A in scCO2 and hexane.
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K. Woelk, September
25, 2000