At 05:21 -0400 16/9/07, Jean-Claude Bradley wrote:
>The issue of shift prediction in different solvent environments could be very 
>useful.  In monitoring reactions by H NMR we have observed significant 
>reproducible shifts over the course of a reaction, presumably because of a 
>change in the composition of the solution.


See my previous post!

By the way, we have tried our protocol on three other natural products.  On
the obtusallenes, we are finalising a paper to  Org Lett on their structural
revision (having had to deal with  Spin Orbit corrections to  13C shifts.  Turns
out that this has a small impact on TMS (yes, SO-coupling to  Si can be about
1-2 ppm!!!)  and hence the referencing standards that are used. 

The second example
is also interesting.  I attended an organic chemistry conference during the 
summer.
One plenary lecturer showed a product with stereochemistry that "instinct"
(I really cannot put it more firmly than that) suggested to me was wrong.
A MOPAC calculation revealed the isomer he showed was  about  60 kcal/mol
higher than a more obvious candidate (by the way,the  La Clair hexacyclinol
energy was about  100 kcal/mol higher than the  Rychnovsky structure. Nature
rarely builds that much energy into its biosynthetic pathways, other than of 
course
the  ATP one. No-one has yet mentioned that the structure could have been
questioned on these grounds alone!!).  I calculated the 13C shifts for
my proposed structure, and now eagerly await to learn if they match
that measured (along with the one shown in the lecture).  Come the day
soon when  ALL of this will be doable on an  iPhone!!  (I am not jesting
by the way).

The third example is perhaps potentially typical as well.  A student
at  Imperial has spent  3 years making a natural product. Of  course, the
penultimate step refused to crystallise, and two diastereoisomers are
isolated.  They do not know which is the correct one.  The 13C
prediction will almost certainly reveal the answer.
-- 

Henry Rzepa.
+44 (020) 7594 5774 (Voice); +44 (0870) 132 3747 (eFax); [EMAIL PROTECTED] 
(iChat)
 http://www.ch.ic.ac.uk/rzepa/ Dept. Chemistry, Imperial College London, SW7  
2AZ, UK.

(Voracious anti-spam filter in operation for received email.
If expected reply not received, please phone/fax).


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