Enantioselective hydrogenation over cinchona-modified Pt: the special role of carboxylic acids

Chemistry. 2002 Mar 15;8(6):1430-7. doi: 10.1002/1521-3765(20020315)8:6<1430::aid-chem1430>3.0.co;2-k.

Abstract

The influence of acetic acid (AcOH) and trifluoroacetic acid (TFA) on the hydrogenation of ethyl-4,4,4-trifluoroacetoacetate has been investigated by using Pt/Al(2)O(3) modified by cinchonidine and O-methylcinchonidine. We have shown that the sometimes dramatic changes in enantioselectivity and rate cannot simply be interpreted by protonation of the alkaloid modifier. We propose a new three-step reaction pathway, involving interaction of the carboxylic acid with the reactant and the chiral modifier. The mechanism is supported by IR spectroscopic identification of cyclic TFA-modifier ion pairs. This new approach can rationalise the poorly understood role of acids in the enantioselective hydrogenation of activated ketones over cinchona-modified platinum metals.