CCL:G: keto-enol-problems



 Sent to CCL by: Andrew Yeung [andrew.yeung,,chem.tamu.edu]
 
Just a thought. In the gas phase, the oscillating hydrogen species is probably the TS of the isomerization.
 In solution state, trace acid or base should catalyze the tautomerization?
 Andrew Yeung
 Donald J. Darensbourg Research Group
 Department of Chemistry, Texas A&M University
 3255 TAMU
 College Station, TX 77843-3255
 Tel: 979 845 4837
 On 2012-06-05 5:11 AM, Ernst Horkel ehorkel(!)ioc.tuwien.ac.at wrote:
 
 Sent to CCL by: "Ernst  Horkel" [ehorkel : ioc.tuwien.ac.at]
 Dear all,
 I have a (at least to me) strange problem when I try to describe a keto-enol
 tautomerism. The substance under inverstigation is a beta-keto carboxylic acid
 amide derivative; there is one possible keto-tautomer (having the ketone and the
 amide a C=O bond). Between the two possible enol-tautomers (one having the O-H
 on carbon C3 and the other having the O-H on the amide C1), there should be a
 transition state; I thik I found it, being planar in geometry with the hydrogen
 oszillating between the two oxygen atoms. A frequency run returned one single
 imaginary frequency with v=-1086cm-1. So this seems to make sence to me, right?
 But now the problem: in order to get the both tautomers connected via this TS, I
 followed the imag.freq. in both directions (manual displacement in gauss view,
 both in positive and negative direction) and optimized those structures. Results
 are chemically correct tautomers, frequency runs showed no imaginary frequency.
 BUT: in one of the tautomers, the gi!
   bbs free energy is HIGHER than in the TS! How is this possible? Does that make
 sence (I don't think so). Please help me and leave comments on this, as I'm
 really stucking at this point for a while.
 some background:
 *planned investigation: realative stability of two tautomers; calculation of the
 activation energy of the tautomerization.
 *used software: Gaussian 09, GaussView 5.0 on a Linux system
 *level of theory: DFT, M06-2X, 6-311G(d,p)++, solvent H2O, PCM theory
 *input (representative): "opt=tight freq 6-311++g(d,p) scrf=(solvent=water)
 geom=connectivity int=ultrafine m062x"
 *for calculation of "delta G" I used the calculated values in the
 ".log" file printed in the line (e.g.): "Sum of electronic and
 thermal Free Energies=         -670.274904"
 So please can anyone help (guide) me out of this. Any helpful ideas or comments
 are really welcome.
 Thank You all in advance,
 best reagrds
 Ernst>